development of innovative bioassay principles for

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DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR PHARMACEUTICAL QUALITY CONTROL - ENTWICKLUNG INNOVATIVER BIOASSAYPRINZIPIEN FÜR DIE PHARMAZEUTISCHE QUALITÄTSKONTROLLE Der Naturwissenschaftlichen Fakultät der Friedrich-Alexander-Universität Erlangen-Nürnberg zur Erlangung des Doktorgrades Dr. rer. nat. vorgelegt von Cornelia Andrea Zumpe aus Nürnberg

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Page 1: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

DDEEVVEELLOOPPMMEENNTT OOFF IINNNNOOVVAATTIIVVEE BBIIOOAASSSSAAYY PPRRIINNCCIIPPLLEESS FFOORR

PPHHAARRMMAACCEEUUTTIICCAALL QQUUAALLIITTYY CCOONNTTRROOLL

--

EENNTTWWIICCKKLLUUNNGG IINNNNOOVVAATTIIVVEERR BBIIOOAASSSSAAYYPPRRIINNZZIIPPIIEENN FFÜÜRR DDIIEE

PPHHAARRMMAAZZEEUUTTIISSCCHHEE QQUUAALLIITTÄÄTTSSKKOONNTTRROOLLLLEE

Der Naturwissenschaftlichen Fakultät

der Friedrich-Alexander-Universität Erlangen-Nürnberg

zur

Erlangung des Doktorgrades Dr. rer. nat.

vorgelegt von

Cornelia Andrea Zumpe

aus Nürnberg

Page 2: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

Als Dissertation genehmigt von der Naturwissenschaftlichen Fakultät

der Friedrich-Alexander-Universität Erlangen-Nürnberg

Tag der mündlichen Prüfung: 26. November 2010

Vorsitzender der Promotionskommission: Prof. Dr. Rainer Fink

Erstberichterstatter: Prof. Dr. Monika Pischetsrieder

Zweitberichterstatter: PD Dr. Dr. Veit J. Erpenbeck

Page 3: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

Danksagung

Die vorliegende Arbeit entstand unter der Anleitung von Prof. Dr. Monika Pischetsrieder am Institut

für Pharmazie und Lebensmittelchemie der Friedrich-Alexander-Universität Erlangen Nürnberg.

Die Arbeit wurde überwiegend bei der Firma Merck Serono in Darmstadt durchgeführt.

Zuerst möchte ich mich bei Prof. Dr. Monika Pischetsrieder für die Bereitschaft, meine Betreuung

seitens der Universität zu übernehmen, bedanken. Ich danke ihr für ihre Unterstützung und

hilfreichen Vorschläge.

Mein besonderer Dank geht an Dr. Christiane Bachmann und Dr. Nicole Wiedemann für die

fachlich kompetente Betreuung dieser Arbeit mit zahlreichen Anregungen und interessanten

Diskussionen. Vielen Dank für die Bereitstellung des spannenden Themas sowie ihr stetiges

Engagement, das erheblich zum Gelingen dieser Arbeit beigetragen hat.

PD Dr. Dr. Veit J. Erpenbeck möchte ich für die Übernahme des Zweitguachtens, sowie seine

interessanten Anregungen danken.

Prof. Dr. Kreis und Prof. Dr. Fromm danke ich für die Bereitschaft, mich in meiner

Promotionsprüfung zu prüfen.

Vielen Dank auch an Dr. Katrin Engel für ihre hilfreichen Ratschläge und stetige

Diskussionsbereitschaft.

Allen aktuellen und ehemaligen Doktoranden von Merck Serono, insbesondere Thomas Lange,

Annette Eppler, Kathrin Ziegler und Maria Leonor Alvarenga danke ich für die gute

Arbeitsatmosphäre und den Spaß bei der Arbeit.

Bei den Mitarbeitern von ADB5, Claudia Fischer, Anke Breuer, Jasmin Oestreicher und Simone

Hartl möchte ich mich für die Einarbeitung in die Zellkultur sowie die Pflege meiner Zellen während

meiner Abwesenheit bedanken.

Herzlichen Dank auch an die Laboratorien von Dr. Ralph Lindemann und Dr. Heike Dahmen für die

Möglichkeit, ihr Odyssey Infrared Imaging System und ihr FACScan Flow Cytometer benutzen zu

dürfen. Bei Melanie Daniel und Doreen Zickler möchte ich mich für die Einweisung in die Geräte

bedanken.

Desweiteren danke ich Enrico Tucci (National Institute of Statistics, Rome, Italy) für die statistische

Auswertung meiner Daten, sowie Francesco Antonetti und Beatrice Brunkhorst (beide Merck

Serono) für das Korrekturlesen meiner Artikel.

Page 4: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

Danken möchte ich auch der Firma Merck Serono für die Finanzierung meiner Arbeit sowie der

Bereitstellung eines Arbeitsplatzes und der erforderlichen Arbeitsmittel.

Zum Schluss möchte ich mich ganz besonders herzlich bei meinen Eltern für die finanzielle und

moralische Unterstützung meines bisherigen Lebensweges bedanken. Danke für ihre Geduld, ihr

Vertrauen und ihren Rückhalt in allen Lebenssituationen.

Page 5: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

TTAABBLLEE OOFF CCOONNTTEENNTTSS

LIST OF ABBREVIATIONS ..................................................................................................................10

LIST OF PUBLICATIONS .....................................................................................................................14

II.. IINNTTRROODDUUCCTTIIOONN .................................................................................................................................................................................................................... 1155

1. OVERVIEW OF THE IMMUNE SYSTEM ..............................................................................................15

1.1. Innate immunity .................................................................................................................15

1.2. Adaptive immunity ............................................................................................................16

1.2.1. Lymphocytes ............................................................................................................... 16

1.2.1.1. B Lymphocytes ..................................................................................................... 16

1.2.1.2. T Lymphocytes ...................................................................................................... 17

1.2.2. APCs ........................................................................................................................... 18

1.4. Cytokines ...........................................................................................................................18

1.4.1. General information ..................................................................................................... 18

1.4.2. Classification and features of cytokines ...................................................................... 19

2. INTERLEUKIN-7, ITS SIGNAL TRANSDUCTION PATHWAYS AND APPLICATION IN IMMUNOTHERAPY .......21

2.1. IL-7 ......................................................................................................................................21

2.2. IL-7R ...................................................................................................................................22

2.3. IL-7 Signal transduction pathways ..................................................................................23

2.3.1. JAK/STAT pathway ..................................................................................................... 25

2.3.2. PI3K/AKT pathway ...................................................................................................... 26

2.3.3. Ras/Raf/ERK pathway ................................................................................................. 27

2.3.4. SFK pathway ............................................................................................................... 27

2.4. IL-7 and cell cycle .............................................................................................................28

2.5. Lymphotrophic effects of IL-7 .........................................................................................28

2.5.1. Induction of anti-apoptotic factors ............................................................................... 28

2.5.2. Suppression of pro-apoptotic proteins......................................................................... 29

2.5.3. Regulation of metabolism: glucose ............................................................................. 29

2.5.4. Regulation of metabolism: pH ..................................................................................... 30

2.6. IL-7 in immunotherapy ......................................................................................................30

3. QUALITY CONTROL OF BIOPHARMACEUTICALS ...............................................................................32

3.1. General remarks about quality control ...........................................................................32

3.2. Criterions for quality control of biopharmaceuticals ....................................................32

3.2.1. Physicochemical properties ......................................................................................... 32

3.2.2. Biological activity ......................................................................................................... 33

3.2.3. Immunochemical properties ........................................................................................ 33

3.2.4. Purity, impurities and contaminants ............................................................................ 33

3.2.5. Quantity ....................................................................................................................... 34

3.3. Biological assays ..............................................................................................................34

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3.3.1. Assay formats and requirements for use in QC .......................................................... 34

3.3.1.1. Overview of assay formats ................................................................................... 34

3.3.1.2. Requirements for use in QC ................................................................................. 35

3.3.2. Analysis models for potency assays ........................................................................... 36

3.3.2.1. The parallel line model .......................................................................................... 36

3.3.2.2. Logistic models (4-and 5-parameter fit) ................................................................ 37

3.3.3. Read-out system for proliferation assays .................................................................... 38

3.3.3.1. Colorimetric detection ........................................................................................... 38

3.3.3.2. Fluorescence ........................................................................................................ 39

3.3.3.3. Luminescence ....................................................................................................... 40

3.4. Investigated biopharmaceuticals ....................................................................................40

3.4.1. Cetuximab (Erbitux®) .................................................................................................. 40

3.4.2. Tucotuzumab celmoleukin (KS-IL2) ............................................................................ 41

3.4.3. Fc-IL7 .......................................................................................................................... 41

IIII.. AAIIMM OOFF TTHHIISS SSTTUUDDYY ...................................................................................................................................................................................................... 4422

IIIIII.. MMAATTEERRIIAALLSS AANNDD MMEETTHHOODDSS ........................................................................................................................................................................ 4433

1. MATERIALS ..................................................................................................................................43

1.1. Cell lines ............................................................................................................................43

1.2. Investigated biopharmaceuticals ....................................................................................44

1.2.1. Cetuximab (Erbitux®) .................................................................................................. 44

1.2.2. Tucotuzumab celmoleukin (KS-IL2) ............................................................................ 44

1.2.3. Fc-IL7 .......................................................................................................................... 44

1.3. Antibodies ..........................................................................................................................44

1.3.1. Primary antibodies ....................................................................................................... 44

1.3.1. Secondary antibodies .................................................................................................. 45

1.4. Controls .............................................................................................................................45

1.4.1. Cell control extracts ..................................................................................................... 45

1.4.2. Isotype controls ........................................................................................................... 46

1.5. Culture medium, reagents and chemicals ......................................................................46

1.6. Composition of buffer & reagent solutions ....................................................................47

1.7. Equipment ..........................................................................................................................48

1.8. Plastic ware and other materials .....................................................................................49

1.9. Software .............................................................................................................................49

2. METHODS ....................................................................................................................................50

2.1. Cell culture .........................................................................................................................50

2.1.1. CTLL-2 cells ................................................................................................................ 50

2.1.2. DiFi cells ...................................................................................................................... 50

2.1.3. Kit 225 cells ................................................................................................................. 50

2.1.4. PB-1 cells .................................................................................................................... 50

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2.1.5. 2E8 cells ...................................................................................................................... 50

2.2. Determination of the cell density ....................................................................................50

2.3. Thawing of cells ................................................................................................................51

2.4. Potency assays (colorimetric proliferation assays) ......................................................51

2.4.1. Principles ..................................................................................................................... 51

2.4.1.1. CTLL-2 potency assay .......................................................................................... 51

2.4.1.2. DiFi potency assay................................................................................................ 51

2.4.2.1. Kit 225 potency assay ........................................................................................... 51

2.4.2. Protocols ...................................................................................................................... 52

2.4.2.1. CTLL-2 potency assay .......................................................................................... 52

2.4.2.2. DiFi potency assay................................................................................................ 52

2.4.2.3. Kit 225 potency assay ........................................................................................... 53

2.4.3. Data evaluation: comparison of different analysis models .......................................... 53

2.4.4. Adaption of assay parameters to luminescence and fluorescence techniques .......... 54

2.5. STAT5 phosphorylation assay ........................................................................................55

2.5.1. Principle ....................................................................................................................... 55

2.5.2. Protocol ....................................................................................................................... 55

2.6. Western blotting analysis.................................................................................................56

2.5.1. Principle ....................................................................................................................... 56

2.5.2. Protocol ....................................................................................................................... 56

2.7. Inhibition with WP1066 .....................................................................................................57

2.7.1. Principle ....................................................................................................................... 57

2.7.2. Protocol ....................................................................................................................... 57

2.8. Flow cytometric analysis .................................................................................................57

2.8.1. Principle ....................................................................................................................... 57

2.8.2. Protocol ....................................................................................................................... 57

IIVV.. RREESSUULLTTSS AANNDD DDIISSCCUUSSSSIIOONN........................................................................................................................................................................ 5588

1. COMPARISON OF DIFFERENT ANALYSIS MODELS (PARALLEL LINE, 4-AND 5-PARAMETER FIT) FOR

POTENCY ASSAYS ............................................................................................................................58

1.1. CTLL-2 potency assay ......................................................................................................58

1.1.1. Concentration ranges .................................................................................................. 58

1.1.2. Test on the necessity of “weighting” ............................................................................ 60

1.1.3. Results ......................................................................................................................... 63

1.2. DiFi potency assay ............................................................................................................69

1.2.1. Concentration ranges .................................................................................................. 69

1.2.2. Test on the necessity of “weighting” ............................................................................ 70

1.2.3. Results ......................................................................................................................... 73

1.3. Combined discussion of CTLL-2 and DiFi potency assays results .............................78

1.4. Summary and Conclusions ..............................................................................................82

Page 8: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

2. COMPARISON OF DIFFERENT PROLIFERATION ASSAYS (COLORIMETRIC, LUMINESCENCE AND

FLUORESCENCE READ-OUTS) ............................................................................................................84

2.1. Method development ........................................................................................................84

2.2. Results ...............................................................................................................................85

2.2.2. CTLL-2 potency assay................................................................................................. 85

2.2.3. DiFi potency assay ...................................................................................................... 91

2.2.4. Kit 225 potency assay ................................................................................................. 94

2.3. Combined discussion of CTLL-2, DiFi and Kit 225 assay results ................................99

2.4. Conclusions .....................................................................................................................101

3. CHARACTERIZATION OF THE IL-7 SIGNAL TRANSDUCTION PATHWAYS AND SELECTION OF AN

APPROPRIATE TARGET FOR DEVELOPMENT OF AN INTRACELLULAR PHOSPHORYLATION ASSAY ..........102

3.1. Results and Discussion of flow cytometric analyses .................................................103

3.2. Results and Discussion of western blotting analyses ................................................106

3.2.1. Representative targets of the JAK/STAT pathway: STAT1, STAT3, STAT5, pim-1 and

bcl-2 ..................................................................................................................................... 106

3.2.1.1. STAT1 and STAT3.............................................................................................. 106

3.2.1.2. STAT5 ................................................................................................................. 108

3.2.1.3. Inhibition of STAT5 by WP1066 .......................................................................... 109

3.2.1.4. Pim-1 ................................................................................................................... 111

3.2.1.5. Bcl-2 .................................................................................................................... 112

3.2.2. Representative target of the PI3K/AKT pathway: AKT .............................................. 114

3.2.3. Representative targets of the ERK pathway: ERK and Bim...................................... 115

3.2.3.1. ERK ..................................................................................................................... 115

3.2.3.2. Bim ...................................................................................................................... 117

3.2.4. Representative target of the SFK pathway: Lck ........................................................ 118

3.2.5. Representative target of the p38 MAPK stress pathway: p38 MAPK ....................... 120

3.3. Summary and Conclusions ............................................................................................121

4. DEVELOPMENT OF A STAT5 PHOSPHORYLATION ASSAY AS AN ALTERNATIVE TO THE CLASSICAL

PROLIFERATION ASSAYS .................................................................................................................124

4.1. Assay development and optimization ...........................................................................124

4.2. Assay qualification .........................................................................................................133

4.3. Comparison of the STAT5 phosphorylation assay to the proliferation assay .........134

4.4. Conclusions .....................................................................................................................134

VV.. OOVVEERRAALLLL CCOONNCCLLUUSSIIOONNSS AANNDD OOUUTTLLOOOOKK........................................................................................................................ 113366

LIST OF FIGURES ...........................................................................................................................138

LIST OF TABLES .............................................................................................................................141

REFERENCES .................................................................................................................................142

APPENDIX: .....................................................................................................................................156

STATISTICAL ANALYSIS OF BIOASSAY RESULTS: A COMPARISON BETWEEN DIFFERENT CALCULATION

MODELS .........................................................................................................................................156

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1. Objective .............................................................................................................................157

2. Definitions ...........................................................................................................................157

3. Statistical Method ..............................................................................................................157

4. Statistical evaluation .........................................................................................................158

4.1. Results of the analyses by Model ................................................................................. 158

4.1.1. CTLL-2 potency assay ........................................................................................... 158

4.1.2. DiFi potency assay................................................................................................. 161

4.1.3. Conclusions ........................................................................................................... 163

4.2. Results of the analyses by Concentration .................................................................... 166

4.2.1. CTLL-2 potency assay ........................................................................................... 166

4.2.2. DiFi potency assay................................................................................................. 168

4.2.3. Conclusions ........................................................................................................... 171

4.3. Results of the analyses by Range ................................................................................ 171

4.3.1. CTLL-2 potency assay ........................................................................................... 171

4.3.2. DiFi potency assay................................................................................................. 174

4.3.3 Conclusions ............................................................................................................ 176

5. Analysis on failure rates....................................................................................................177

5.1 CTLL-2 potency assay................................................................................................... 178

5.2 DiFi potency assay ........................................................................................................ 179

5.3 Conclusions ................................................................................................................... 180

ABSTRACT .....................................................................................................................................181

ZUSAMMENFASSUNG ......................................................................................................................182

CURRICULUM VITAE .......................................................................................................................184

Page 10: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

LIST OF ABBREVIATIONS

4PL Four-parameter fit

5PL Five-parameter fit

ADCC Antibody-dependent cellular cytotoxicity

ADP Adenosine di-phosphate

AIT adoptive immunotherapy

AML Acute myeloid leukemia

ANOVA ANalysis Of VAriance

AP Activator protein

APC Antigen-presenting cell

API Active pharmaceutical ingredient

ATCC American Type Culture Collection

ATP Adenosine triphosphate

BCP-ALL B cell precursor acute lymphoblastic leukemia

BCR B cell receptor

BSA Bovine serum albumin

CD Cluster of Differentiation

CDK Cyclin dependent kinase

CHK Checkpoint kinase

CKI Cyclin dependent cell cycle inhibitor

CLP Common lymphoid progenitor

CRC Colorectal cancer

C test Cochran‟s test

CTL Cytotoxic T lymphocytes

CV Coefficient of variation

DC Dendritic cells

DMSO dimethyl sulfoxide

DNA Desoxy-ribonucleic acid

DPBS Dulbecco‟s Phosphate-Buffered Saline

DSMZ Deutsche Sammlung von Mikroorganismen und Zellkulturen

(German collection of microorganisms and cell cultures)

DTT dithiothreitol

EC Ethylene carbonate

EBF Early B cell factor

EGFR Epidermal Growth Factor Receptor

ELISA Enzyme-linked immuno sorbent assay

EMD Emanuel Merck, Darmstadt

EMSA Electrophoretic Mobility Shift Assay

EpCAM Epithelial cell adhesion molecule

Page 11: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

ERK Extracellular-signal regulated kinase

ETC Electron transport chain

FACS Fluorescence Activated Cell Sorting

FBS Fetal bovine serum

FDA Food and Drug Administration

GI Gastro-intestinal

GLUT Glucose transporter

GMP Good manufacturing practice

GSK-3 Glycogen synthase kinase-3

h hour

HBSS Hank‟s Buffered Salt Solution

HIV Human immunodeficiency virus

HLA Human leukocyte antigens

HRP Horseradish peroxidase

hu human

ICH International Conference on Harmonization

IFN Interferon

Ig Immunoglobulin

IL Interleukin

IL-7R IL-7 receptor

IR Infrared

IRS Insulin receptors

iT-Reg cells Induced T-Reg cells

JAK Janus Kinase

JNK Jun N-terminal kinases

kDa Kilo Dalton

KIRA KInase Receptor Activation

KS test Kolmogorov-Smirnov test

KW test Kruskal-Wallis test

LAK cell Lymphokine activated killer cell

L test Levene‟s test

MAPK Mitogen-activated protein kinase

MCL myeloid leukemia cell differentiation protein

ME β-mercaptoethanol

MHC Major histocompatibility complex

min minute

mRNA messenger ribonucleic acid

MTS/ PMS (3-(4,5-dimethylthiazol-2-yl)-5-(3-carboxymethoxyphenyll-2-(4-

sulfophenyl)-2 H-tetrazolium, inner salt)/phenazine methosulfate)

MTT (3-(4,5-Dimethylthiazol-2-yl)-2,5-diphenyltetrazoliumbromid)

Page 12: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

mu murine

NAD Nicotinamid-adenin-dinucleotid

NBE New Biological Entity

Neg. C. Negative control

NHE sodium/hydrogen exchanger

NK cell Natural killer cell

NSCLC Non-small cell lung carcinoma

nT-Reg Natural T-Reg cells

OD Optical density

p- Phospho-

PAGE Polyacrylamide gelelectrophoresis

PAMP Pathogen-associated molecular pattern

PE Phycoerythrin

Ph. Eur. European Pharmacopeia

PI3K Phosphatidylinositol 3-kinase

PIP Phosphatidylinositol-4,5-bisphosphate

PL model Parallel line model

Pos. C. Positive control

PPBSF Pre-pro-B cell growth-stimulating factor

PVDF Polyvinylidenefluoride

QC Quality control

Rb Riboblastoma

RE Relative error

RFU Relative fluorescence units

RLU Relative light units

rpm Rounds per minute

RT Room temperature

SCF Stem cell factor

SCLC Small cell lung carcinoma

SCID Severe combined immunodeficiency syndrome

SD Standard deviation

SDS Sodium dodecyl sulfate

SFK Src family kinase

SIV Simian immunodeficiency virus

SOCS Suppressor of cytokine signaling

SOP Standard operation procedure

SH Src homology

Shc Src homology and collagen

STAT Signal Transducer and Activator of Transcription

TCR T cell receptor

Page 13: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

TGF-β Tumor growth factor-β

TH cells T helper cells

TMB Tetramethyl benzidine

TNF Tumor necrosis factor

T-Reg cells Regulatory T cells

USP United States Pharmacopeia

WB Western blotting

XSCID X-linked severe combined immunodeficiency

XTT (sodium(2,3-bis(2-methoxy-4-nitro-5-sulfophenyl~-2H-tetrazolium-5-

carboxanilide)

Page 14: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

LIST OF PUBLICATIONS

Parts of this work have already been published or submitted:

A. Full research papers

Zumpe C., Wiedemann N., Metzger A.U., Pischetsrieder M., Bachmann C.L. Analysis of

potency assays: comparison between the parallel line method and logistic models (four-and

five-parameter fit). J. Pharm. Biomed. Anal., 2010, under revision.

Zumpe C., Bachmann C.L., Metzger A.U., Wiedemann N. Comparison of potency assays

using different read-out systems and their suitability for quality control. J. Immunol.

Methods, 360 (2010) 129-140.

Zumpe C., Engel K., Wiedemann N., Metzger A.U., Pischetsrieder M., Bachmann C.L.

Development of a STAT5 phosphorylation assay as a rapid bioassay to assess Interleukin-

7 potency. Curr. Pharm. Biotech, 2010, under revision.

Zumpe C., Engel K., Wiedemann N., Metzger A.U., Pischetsrieder M., Bachmann C.L.,

Interleukin (IL)-7 and IL-2 signaling in human T and murine B cell lines. Cell. Signal. 2010,

submitted.

B. Posters and oral presentations

Zumpe C., Wiedemann N., Metzger A.U., Pischetsrieder M., Bachmann C.L., Analysis of

potency assays: comparison between the parallel line method and logistic models (four-and

five-parameter fit). Presented at BEBPA's 1st Inaugural Biological Assays Conference, Sept

10-12, 2008, Berlin, Germany.

Zumpe C., Bachmann C.L., Metzger A.U., Wiedemann N., Comparison of potency assays

using different read-out systems and their suitability for quality control. Presented at

BEBPA„s 2nd

Inaugural Biological Assays Conference, Sept 30 – Oct 2 2009, Rome, Italy

and at the “DPhG Doktorandentagung”, Nov 18-21, Pichlarn, Austria.

Page 15: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

I. INTRODUCTION

15

II.. IINNTTRROODDUUCCTTIIOONN

In the following section, first, a short overview about the immune system and its components will be

given. Special focus will be drawn on cytokines and especially on Interleukin (IL)-7. IL-7 and other

cytokines are often used in combination with parts of antibodies for anti-cancer therapies. Quality

control of those biopharmaceuticals is usually achieved by using biological assays, which will be

discussed in the second part of this introduction.

1. OVERVIEW OF THE IMMUNE SYSTEM

In order to efficiently resist against pathogens like viruses, bacteria and parasites, mammalians

developed a complex immune system. This system is composed of two major subdivisions, the

innate or non-specific immune system and the adaptive or specific immune system (Janeway and

Travers, 1994). The innate immune system provides the first line of defense against pathogens,

while the adaptive immune system acts as a second line of defense, displaying a high degree of

antigen-specificity and affording protection against re-exposure to the same pathogen (Male et al.,

2006). An interaction and well functioning of both parts is required for a successful resistance

against infections.

1.1. Innate immunity

Recognized as the first line of defense, the innate immune system consists of anatomic,

physiological, phagocytic or endocytic, as well as inflammatory barriers.

The skin and internal epithelial layers act as mechanical, anatomic barriers against invading

pathogens. Associated with these protective surfaces are chemical and biological agents, e.g.

defensins and surfactants.

The humoral or physiological barriers consist of various different factors, e.g. lysozymes, which are

cleaving bacterial cell walls, interferons, which can limit virus replication in cells, as well as

lactoferrin and transferrin, which inhibit bacterial growth by binding iron, an essential nutrient for

bacteria. The major humoral non-specific defense mechanism is the complement system, a

multicomponent triggered enzyme cascade. Once activated, complement can lead to increased

vascular permeability, recruitment of phagocytic cells, as well as lysis and opsonization of bacteria.

The phagocytic or endocytic barrier of the innate immune system consists of a variety of cells of the

innate immune system, which are recruited to the sites of infection, beyond them natural killer (NK)

cells, macrophages, neutrophils and eosinophils. These cells are the main line of defense in the

non-specific immune system and exert different activities. NK and lymphokine activated killer (LAK)

cells can nonspecifically kill virus infected and tumor cells, whereas eosinophils can kill certain

parasites by releasing proteins from granula. Neutrophils can phagocytose invading organisms and

kill them intracellularly. Macrophages contribute to intracellular as well as to extracellular killing of

microorganisms, infected and altered self target cells. Furthermore, macrophages can repair tissue

and act as antigen-presenting cells (APCs), which are required for the induction of specific immune

responses.

Page 16: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

I. INTRODUCTION

16

The inflammatory response is a complex sequence of events that is caused by tissue damage or

invading pathogenic microorganisms and leads to vasodilatation, increased capillary permeability

and influx of phagocytic active cells from capillaries into the tissue (Male et al., 2006; Goldspy,

2000; Murphy, 2008).

In addition to the activities described above, the innate immune system is also responsible for the

initial release of cytokines and chemokines that activate the adaptive immune system. The role of

cytokines will be further discussed in section I.1.3.

1.2. Adaptive immunity

If the effector mechanisms of the innate immune system fail to eliminate the invading pathogens,

the components of the specific or adaptive immune system are activated. Adaptive immunity is

characterized by antigen specificity and is capable of recognizing and selectively eliminating

specific foreign microorganisms and molecules (Roitt, 1994). This specificity is achieved through

usage of clonally distributed antigen receptors, i.e. surface Ig on antibody-producing B lymphocytes

and T cell receptors (TCRs) on the surface of T lymphocytes.

In addition to the antigen-specificity - permitting the immune system to distinguish even slight

differences among antigens - the adaptive immunity is characterized by an enormous diversity of

recognition molecules that can be generated. This represents an immunologic memory that

enables the immune system to respond to previously encountered antigens with a higher reactivity.

Adaptive immune responses can be divided into humoral and cell-mediated responses. Humoral

responses involve the interaction of B lymphocytes/cells, T lymphocytes/cells and APCs, whereas

cell-mediated responses need the cooperation of different subclasses of T cells, macrophages and,

to a lesser extent, NK cells (Dawson et al., 1996).

1.2.1. Lymphocytes

Lymphocytes are divided into B and T lymphocytes, exerting different, specific functions in the

immune system. They express specific receptors, the T and B cell antigen receptors (BCRs), which

are responsible for the enormous diversity of T and B cells and are able to discriminate between

self and non-self.

1.2.1.1. B Lymphocytes

B lymphocyte progenitors arise from hematopoietic stem cells and differentiate to B lymphocytes in

the bone marrow. During maturation, B cells go through several stages which are characterized by

changes in the rearrangement of Ig heavy and light chain genes and intracellular as well as surface

marker expression. After maturation, B cells migrate from the bone marrow to the B cell zone in

secondary lymphoid organs, such as the spleen and lymph nodes. On their surface, B cells

express the BCR, recognizing the native form of an antigen. By interaction with an antigen, B cells

start to proliferate and differentiate into effector B cells and produce and secrete large amounts of

antigen-specific memory B cells and effector plasma cells, which generate large amounts of soluble

but otherwise identical versions of the membrane-bound Ig (Abbas et al., 1996).

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This clonal selection hypothesis (Talmage, 1986) explains why subsequent responses to the same

antigen are more effective and long-lasting as in the initial response (Dawson et al., 1996). In the

first encounter with an antigen, a primary antibody response is generated; later, a re-encounter with

the same antigen causes a more rapid secondary response, producing high levels of antibodies

with a high binding affinity for the target antigen. This process is also exploited in prophylactic

vaccination.

1.2.1.2. T Lymphocytes

T lymphocyte progenitors arise from hematopoietic stem cells in the bone marrow and migrate to

the thymus to mature. T lymphocytes express the TCR, recognizing only processed antigen

peptides bound to the major histocompatibilty complex (MHC). In contrast to B cells, T cells do not

identify native, unbound antigens. It can thus be avoided that cytotoxic T cells directly lyse own

cells.

During maturation, TCRs with too low or too high affinity for MHC molecules are deleted in a two-

step selection process in the thymus. Positive selection of T cells ensures that mature TCRs bind

to self-MHC molecules which confers MHC restriction (Zinkernagel et al., 1974). T cells with high

affinity for self-MHC molecules or self-MHC plus self-antigen undergo negative selection which

ensures self-tolerance. T cells that fail positive selection or get negatively selected during

maturation die by apoptosis. After maturation, T cells can be divided into two distinct populations

depending on their functional phenotype and expression of the Cluster of Differentiation (CD)4 or

CD8 co-receptor.

CD4+ T helper cells (TH cells) are specific for antigenic peptides presented by MHC class II

molecules and upon activation, proliferate and secrete various cytokines which in turn activate B

cells, T cells, macrophages and other cells involved in the immune response.

TH cells can be classified into TH1 and TH2 cells. The differentiation of these subsets from Th0

precursor cells is driven by cytokines, especially by IL-12/IL-18 and IL-4, respectively (Kaufmann,

2002). The TH1 subset supports inflammation by secreting IL-2, interferon (IFN) -γ and tumor

necrosis factor (TNF) -ß and is responsible for classical cell-mediated functions involving CD8+ T

cells. TH2 cells produce IL-4, IL-5 and IL-10 and thus support mainly humoral immune responses

involving B cell proliferation and differentiation into antibody-secreting plasma cells and memory

cells (Mosmann, 2002).

Other groups of TH cells include the regulatory T (T-Reg) and TH-17 cell populations. T-Regs with

the phenotype CD4+CD25

+, usually secrete IL-10 and tumor growth factor-β (TGF-β). Reductions in

T-Reg cells may contribute to autoimmunity, chronic viral infection, tumor immunity and allergy

while the role of the pro-inflammatory IL-17 secreting subgroup pertains probably to host defense

and autoimmunity (Bettelli et al., 2007; Schwartz, 2005).

Activated CD8+

cytotoxic T lymphocytes (CTLs) recognize and lyse specifically autologous virus-

infected cells or tumor cells, which present foreign antigenic peptides on MHC class I molecules

(Schöllmann et al., 2004). In contrast to CD4+ T cells, they can only eliminate intracellular

pathogens.

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1.2.2. APCs

Every cell is capable of presenting endogenous antigens on class I MHC complexes whereas only

APC display endogenous as well as exogenous antigens on class I and class II MHC molecules.

The best studied APCs are macrophages, dendritic cells (DC) and B cells, but it has been shown

that 17 other cells such as liver sinusoidal endothelial cells are able to present exogenous antigens

on class II MHC molecules as well (Limmer et al., 2000).

Complexes between antigenic peptides and MHC molecules are formed by degradation of a

protein antigen by two different antigen-processing pathways. Endogenous proteins derived from

normal cells, tumors, viruses or intracellular bacteria are degraded by the proteasome into peptides

and transported into the rough endoplasmic reticulum where they are loaded onto MHC class I

molecules. The peptide-loaded MHC class I molecules present the endogenous peptide to CD8+

CTL. Exogenous antigens are internalized by APC by receptor-mediated endocytosis in all APC

and by phagocytosis and macropinocytosis in DCs and macrophages. Exogenous peptides are

loaded on MCH II molecules and presented to CD4+ T cells (Goldspy, 2000; Murphy, 2008).

1.4. Cytokines

1.4.1. General information

Cytokines are secreted proteins with growth, differentiation, and activation functions that regulate

and determine the nature of immune responses (Commins et al., 2010). They were initially

identified as products of immune cells that act as mediators and regulators of immune processes

but may be produced by other cells than immune cells and have effects on non-immune cells, as

well. Cytokines are currently being used clinically as biological response modifiers for the

treatment of various disorders. The term cytokine is a general term used to describe a large group

of proteins. Sub-classes of cytokines are for example monokines (cytokines produced by

mononuclear phagocytic cells), lymphokines (cytokines produced by activated lymphocytes,

especially TH cells) and interleukins (cytokines that act as mediators between leukocytes) (Male,

2006).

Many cytokines are pleiotropic - that means that they are produced by many different cell types and

act on various cell types - and redundant - e.g. they exert similar mechanisms of action.

Redundancy is due to the nature of the cytokine receptors. Cytokine receptors are usually

heterodimers - and sometimes heterotrimers - that can be grouped into families with common

subunits for a given family. Examples for cytokine families are shown in table 1. The subunit

common to all members of the family is responsible for cytokine binding and signal transduction.

Thus, a receptor for one cytokine can often respond to another cytokine in the same family. An

individual lacking IL-2, for example, is not adversely affected because other cytokines with the

same subunit (IL-15, IL-7, IL-9, etc.) take over its function. Similarly, a mutation in a cytokine

receptor subunit other than the one in common often has little effect. On the other hand, a

mutation in the common subunit has profound effects. For example, a mutation in the gene for the

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IL-2Rγ subunit causes human X-linked severe combined immunodeficiency (XSCID) characterized

by complete or nearly complete T and B cell defects (Male et al., 2006).

Table 1. Survey of cytokine families. Source: Commins et al. (2010)

Family Members

Hematopoietic

Common γ chain IL-2, IL-4, IL-7, IL-9, IL-15, IL-21

Shared β chain (CD131) IL-3, IL-5

Shared IL-2β chain (CD122) IL-2, IL-15

Other hematopoietic IFN-γ, IL-7, IL-13, IL-21, IL-31, TSLP

IL-1 family IL-1α, IL-1β, IL-1rα, IL-18, IL-33

gp130-utilizing IL-6, IL-11, IL-27, IL-31, ciliary neurotrophic factor, cardiotrophin 1, leukemia inhibitory factor, oncostatin M

IL-12 IL-12, IL-23, IL-35

IL-10 superfamily IL-10, IL-19, IL-20, IL-22, IL-24,

IL-26, IL-28, IL-29

IL-17 IL-17A-F, IL-25 (IL-17E)

Interferons

Type I interferons IFN-α, IFN-β, IFN-ω

Type II interferon IFN-γ (also a hematopoietic cytokine)

Type III interferons IFN-λ1 (IL-29), IFN-λ2 (IL-28A), IFN-λ3 (IL-28B)

TNF superfamily TNF-α, TNF-β, BAFF, APRIL

Cytokines often influence the synthesis of other cytokines and vice versa. They can enhance or

suppress production of other cytokines. In addition, they can influence the action of other

cytokines. These effects can be antagonistic, additive or synergistic.

1.4.2. Classification and features of cytokines

Cytokines can be sub-divided into different categories based on their functions or their source.

They can be grouped according to those that are predominantly APC or T lymphocyte derived; that

predominantly mediate cytotoxic (antiviral and anticancer), humoral, cell-mediated (TH1 and TH17),

or allergic immunity (TH2); or that are immunosuppressive (T-Reg) (Commins et al., 2010).

However, it is important to remember that any attempt to categorize them will be subject to

limitations since they can be produced by many different cells and act on many different cells.

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In table 2, the sources, targets and primary effects of some of the most prominent cytokines are

shown.

Table 2. Features of cytokines. Source: Male et al. (2006)

Cytokine Cell Source Cell Target Primary Effects

IL-1 Monocytes Macrophages Fibroblasts Epithelial cells

T cells, B cells Endothelial cells Hypothalamus Liver

Costimulatory molecule Activation (inflammation) Fever Acute phase reactants

IL-2 T cells, NK cells

T cells B cells Monocytes

Growth Growth Activation

IL-3 T cells Bone marrow progenitors

Growth and differentiation

IL-4 T cells Naive T cells T cells B cells

Differentiation into a TH2 cell Growth Activation and growth, Isotype switching to IgE

IL-5 T cells B cells Eosinophils

Growth and activation

IL-6 T cells, Macrophages, Fibroblasts

T cells, B cells Mature B cells Liver

Costimulatory molecule Growth (in humans) Acute phase reactants

IL-8 family

Macrophages, Epithelial cells, Platelets

Neutrophils Activation and chemotaxis

IL-10 T cells (TH2) Macrophages T cells

Inhibits APC activity Inhibits cytokine production

IL-12 Macrophages, NK cells

Naive T cells Differentiation into a TH1 cell

IFN-γ T cells, NK cells Monocytes Endothelial cells Many tissue cells - especially macrophages

Activation Activation Increased class I and II MHC

TGF-β T cells, Macrophages

T cells Macrophages

Inhibits activation and growth Inhibits activation

GM-CSF T cells, Macrophages, Endothelial cells, Fibroblasts

Bone marrow progenitors

Growth and differentiation

TNF-α Macrophages, T cells

Similar to IL-1 Similar to IL-1

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2. INTERLEUKIN-7, ITS SIGNAL TRANSDUCTION PATHWAYS AND APPLICATION IN

IMMUNOTHERAPY

Interleukin-7 (IL-7), also previously termed „„lymphopoietin 1‟‟ or „„pre-B cell factor‟‟, is a pleiotropic

cytokine, which is produced by stromal cells and thymic epithelial cells in lymphoid organs (Jiang et

al., 2005). Namen et al. discovered IL-7 in 1988 as a growth factor for murine pre B cells. Aside

from being an indispensable factor for the survival of lymphocytes, it also plays a decisive role in

the development of murine and human T cells. A loss of IL-7 signaling can thus lead to a severe

combined immunodeficiency syndrome (SCID) (Puel et al., 1998).

The functional role of IL-7 has not yet been fully elucidated. However, it is clear that perturbation of

this system is of biological significance. IL-7 can be fused to proteins and due to its strengthened

effect on the immune system be used in anti-cancer therapies.

2.1. IL-7

The size of the human IL-7 gene is 72kbp and encodes for a protein of 177 amino acids with a

molecular weight of 25 kilo Dalton (kDa). The size of the murine IL-7 gene is in contrast 41kbp and

encodes a 154 amino acids protein of about 18kDa. The active form of human IL-7 is a

glycoprotein, which is predicted to form a four -helix structure with a hydrophobic core (Kroemer

et al., 1996).

The homology between the murine and human amino acids sequences is 55%. The main

difference of the human protein in comparison to the murine one is an insertion of 19 amino acids

close to the C-terminal region, which appears not to be essential for activity (Goodwin et al., 1990).

23 out of the first 25 amino acids in the signal sequence of the N-terminal region are identical for

human and mouse IL-7, which leads to a 92% homology in this region. Consequently, murine IL-7

also binds to the human IL-7 receptor, which was shown by Goodwin et al. (1990).

The actual active form of IL-7 has been supposed to be a heterodimer of IL-7 and a cofactor, the

pre-pro-B cell growth-stimulating factor (PPBSF). This 55kDa complex stimulates proliferation and

differentiation of pre-pro-B cells (McKenna et al., 1998; Lai et al., 1998).

Mature IL-7 contains six cystein residues and might thus lose its biologic activity upon reduction

with thiols, e.g. ß-mercaptoethanol (Henney, 1989). Cosenza et al. (1997) investigated the tertiary

structure of IL-7 by biophysically and genetically mapping the disulfide bonds in human (hu) IL-7

using a combination of MALDI mass spectroscopy and site-directed cysteine to serine mutational

analyses. They found three cysteine residue pairs (Cys3-Cys142, Cys48-Cys93, and Cys35-

Cys130) participating in disulfide bond formation. Amongst them, only one single disulfide bond is

sufficient to retain a biologically active conformation.

The requirement for IL-7 starts from the pro-T1 and T2 cells, over the selection of CD8 cells to the

mature T cell, which also needs IL-7 for survival and homeostatic proliferation (Khaled et al., 2002).

The IL-7 receptor (IL-7R) regulates both early murine lymphocyte differentiation and proliferation. In

contrast, it cannot stimulate the proliferation of mature B cells (Lee et al., 1989).

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However, its pleiotropic effect is not only restricted to cells of the lymphoid lineage since it also

induced an increase in Desoxy-ribonucleic acid (DNA) synthesis in acute myelogenous leukemia

cells (Digel et al., 1991). Moreover, it activates macrophages in vitro (Alderson et al., 1991) and

generates LAK cells (Alderson et al., 1990).

2.2. IL-7R

IL-7 acts by binding to the IL-7R (see figure 1),

which consists of the IL-7 receptor chain (IL-

7R , CD127) and the common cytokine c chain

( c) that is also shared by the receptors for IL-2,

IL-4, IL-9, IL-15, and IL-21 (Kovanen et al., 2004).

The sequence of the extracellular domain of IL-

7R resembles thus those of other cytokine

receptors as well as those of the prolactine and

growth hormone receptors (Goodwin et al., 1990).

IL-7R belongs to the type I cytokine receptor

family. As a consequence, also the signal

transduction pathways of IL-7 are supposed to

resemble those of other cytokines, especially IL-

2. However, in contrast to IL-2R, IL-7R does not

contain a β-chain.

IL-7R is a membrane glycoprotein with a calculated weight of 49.5kDa. The observed weight for

the expressed receptor molecule might however be higher due to glycosylation or other

posttranslational modifications. The human and murine IL-7R show a high degree of homology

(64%) (Goodwin et al., 1990). All six extracellular and four intracellular cystein residues are

conserved in both receptor molecules. Like other hematopoietic growth factors, both have an

unusual distribution of amino acid residues (Moseley et al., 1989) and contain a high number of

serine and proline residues.

A small membrane-proximal domain, termed „„Box1‟‟, can be found in the IL-7R intracellular part,

which is ubiquitous throughout the type I cytokine receptor family (Murakami et al., 1991).

Furthermore, the structure of IL-7R consists of two fibronectin-like domains, four conserved

cysteine residues and a single 25 amino acid transmembrane domain. It has a 195 amino acid

cytoplasmic tail, which is sub-divided in an acidic rich region (A), a serine rich region (S), and a

tyrosine rich region (T) containing three tyrosine residues (Y401, Y449 and Y456) that are

conserved in mouse and man (Porter et al., 2001). Amongst them, the Y449 site is exceptionally

interesting because it is the origin of two fundamental IL-7 signaling pathways, the Janus Kinase

(JAK)/Signal Transducer and Activator of Transcription (STAT) pathway and the

phosphatidylinositol 3-kinase (PI3K)/AKT pathway, described in detail in section I.2.3. (Pallard et

Figure 1. 3D structure of the IL-7 receptor.

The structure of the IL-7R consists of the IL-7R

chain and the common cytokine c chain ( c), which is also shared by other cytokine receptors. Source: http://www.jpkc.yzu.edu.cn/course/yxmyx/ chapter7/il7r.gif, 20.12.09

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al., 1999). The different regions of the cytoplasmic tail (Box1, A, S and T) can serve as docking

sites for different kinases and thus activate various signaling pathways.

IL-7R exists in a low and a high affinity form, showing different binding kinetics (Goodwin et al.,

1990). It is expressed mainly by hematopoietic cells such as B and T lymphocytes as well as by

selected myeloid cells and endothelial cells. IL-7R subsists in membrane-bound and soluble

forms, which can bind IL-7 in solution. Furthermore, the existence of other isoforms, e.g. two

immunologically distinct proteins (p75 and p90) is discussed (Armitage et al., 1992). The structure

of the IL7-R isoforms has however not yet been fully elucidated.

IL-7R expression is negatively regulated by IL-7 and other cytokines (Park et al., 2004). Having

received cytokine-mediated survival signals, both, CD4+ and CD8

+ T cells reduce IL-7R

transcription in order to avoid competition with unactivated T cells for remaining IL-7.

2.3. IL-7 Signal transduction pathways

So far, relatively little is known about the IL-7 signal transduction pathways. The major pathway(s)

may not have been identified yet, but it is presumed to resemble that of other c family cytokines

(Jiang et al., 2005), particularly IL-2. As both exert similar functions, such as stimulation of T cells,

activation of macrophages and generation of LAK cells, their signal transduction pathways might be

analoguoues. However, not all pathways of IL-2 are shared by IL-7. The protein p52shc

is for

example not activated by IL-7 (Dorsch et al., 1994).

Both IL-7R and c are essential for the biological effects of IL-7. Ligand binding leads to the

heterodimerization of the two receptor chains (Ziegler et al., 2005) and activates thus the receptor

associated tyrosine Janus kinases, JAK1 (IL-7R ) and JAK3 ( c) (Suzuki et al., 2000). Thereby,

JAK3 is firstly activated by binding to c and then phosphorylates the chain-associated JAK1 and

the chain itself. As a consequence, docking sites for signaling molecules with Src homology 2

(SH2) domains were created. The most common example for this is STAT5 and to a lesser extent

STAT1 and STAT3 (Yu et al., 1998; Leonard, 2001). Their SH2 domains dock to a phosphorylated

tyrosine residue (e.g. STAT5 binds phospho-Y449 on IL-7R ) and become themselves

phosphorylated. Phosphorylated STATs dimerize and translocate into the nucleus, which leads to

an activation of specific genes (Foxwell et al., 1995). Via association with the scaffolding protein,

Gab2, STAT5 can activate two signaling pathways that are involved in cell proliferation, the

PI3K/AKT and Ras/mitogen-activated protein kinase (MAPK) pathways (Nyga et al., 2005).

However, in contrast to IL-2 and IL-15, IL-7 seems not to activate the Ras/MAPK pathway (Crawley

et al., 1996).

The most important signaling pathways of IL-7 are illustrated in figure 2. Discontinuities in the

pathways are directly associated with a significant decrease of both pre- and mature T cells

(Nosaka et al., 1995; Yao et al., 2006). Thereby, signals starting from Box1 and Y449 seem to be

particularly important since they are essential for IL-7 mediated T cell survival and proliferation

(Jiang et al., 2004). In the following, the different steps of the signaling pathways will be further

described in detail.

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Figure 2. Illustration of the most important IL-7 signaling pathways.

Figure 2 Shows the main signal transduction pathways, which are presumed to be activated by IL-7. All of these pathways are supposed to be activated by IL-2, as well.

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2.3.1. JAK/STAT pathway

JAK3 is considered to be the first step in the signaling pathway of IL-7. It is associated with the

carboxy-terminal region of c and is thus an essential transducer of c-dependent signals (Suzuki

et al., 2000). JAK3 is predominantly expressed in hematopoietic cells and is involved in IL-2, IL-4

and IL-7 receptor signaling. JAK 3 activities protect cells from apoptosis (Eynon et al., 1999; Suzuki

et al., 2000; Wen et al., 2001).

JAK1 is activated by JAK3 after IL-7 treatment. It also seems to be crucial in IL-7 signaling (Rodig

et al., 1998); however, hardly anything is published about its transduction pathways. JAK1 is

associated with the protein tyrosine kinase Pyk2, which is activated by IL-7 incubation and supports

survival of a thymocyte cell line. Furthermore, JAK1 might play a role in IL-7-induced PI3K

activation (Migone et al.,, 1998).

By downregulating JAK1 activation, IL-7 induces negative feedback on its own signaling. IL-7

treatment induces expression of suppressor of cytokine signaling (SOCS) proteins. SOCS proteins

can suppress cytokine signaling by binding and inhibiting JAKs, by competing with STATs on the

receptor docking site, or by targeting signaling proteins for proteasomal degradation (Starr et al.,

1998). The SOCS protein family consists of eight members (SOCS1–7 and CIS) which all include

a central SH2 domain. This SH2 domain binds and inhibits all JAK family members, including

JAK1. Furthermore, JAKs are dephosphorylated by the phosphatase CD45, which plays a major

role in inhibiting the activity of src kinases (Irie-Sasaki et al., 2001).

STATs are activated by JAKs via their transcriptional activation domain at the carboxy-terminus.

Transcriptional activity can be increased by serine phosphorylation within this domain, presumably

by recruiting other transcription factors. Afterwards, the adjacent SH2 domain docks to a

phosphorylated tyrosine residue (e.g. STAT5 binds phospho-Y449 on IL-7R ) and, after being itself

phosphorylated on a specific tyrosine residue, it also mediates dimerization, interacting with other

SH2 domains. In mammalian cells, seven STAT proteins have been identified (Leonard and

O'Shea, 1998). The STATs are localized as clusters on chromosomes: STAT1 and STAT4 on

chromosome 1, STAT2 and STAT6 on chromosome 10, and STAT3, STAT5A and STAT5B on

chromosome 11 in the murine system (Copeland et al., 1995).

IL-7 is supposed to activate STATs 1, 3 and 5 (Jiang et al., 2004). However, only deficiencies in

STAT5 play a crucial role in thymocyte development. IL-7 induces phosphorylation of both isoforms

of STAT5, STAT5A and B. The two isoforms can form homo or heterodimers and show a 96%

homology in their amino acid sequence.

The docking site for STAT5 is tyrosine residue Y449, on the IL-7Rα. Its activation by IL-7 induces

most of the pathways leading to IL-7 mediated survival. STAT5 regulates the expression of several

Bcl-2 family members and caspases and exerts an anti-apoptotic activity (Debierre-Grockiego,

2004). The induction of bcl-2 messenger ribonucleic acid (mRNA) is impeded by a lacking

phosphorylation of STAT5, which occurs as a consequence of mutations of tyrosine 449 in the IL-

7R chain (Kim et al., 2003). However, other pathways like the phosphorylation of the pro-

apoptotic protein Bad are not influenced by blocked STAT5.

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There is considerable evidence that STAT5 is important in T cell development. Furthermore,

STAT5 seems to play a role in adjusting the number of B cell precursors (Sexl et al., 200) and in

regulating the TCR locus accessibility and thus T cell development (Ye et al., 2001).

Phospho-STAT5 binds to the same promoter elements as the B lineage transcription factor, early B

cell factor (EBF), which might thus lead to synergisms causing the expression of Pax5, a critical

transcription factor expressed early in B lineage cells (Corcoran et al., 1998). STAT3/STAT5 can

bind directly to the pim-1 promoter, leading to an up-regulated expression of the serine/threonine

kinase pim-1. Pim-1 itself can negatively regulate the JAK/STAT pathway by binding to SOCS

proteins (Losmann et al., 1999). Upon phosphorylation, the stability of SOCS proteins and

subsequently their inhibitory effect on STATs is increased (Chen et al., 2002). In turn, the

transcriptional activity of STAT5 can be upregulated by an IL-7-induced serine phosphorylation

(Nagy et al., 2002).

The inactivation of STAT5 inhibits the proliferation of some but not all cytokine receptors; however,

the activation of STAT5 may not induce proliferation (Isaksen et al., 2002). It remains thus to be

determined whether STAT5 is required only for survival signaling or also induces cell proliferation.

Furthermore, it remains unclear, whether other pathways are involved in T cell proliferation. In each

case, STAT5 is a key molecule downstream of IL-7R and might eventually even be the most

important signaling pathway of IL-7 (Goetz et al., 2004).

2.3.2. PI3K/AKT pathway

PI3Ks are lipid kinases being important for proliferation and survival of various cell types, e.g. B

and T cell development (Datta et al., 1999). Upon IL-7 stimulation, their p85 subunit binds to the

phosphorylated Y449 residue on the IL-7R chain via an SH domain and activates the catalytic

subunit (Venkitaraman and Cowling, 1994). Mutations of Y449 block PI3K activity and impede

proliferation of B cells (Corcoran et al., 1996).

The downstream mediators of PI3K have not been fully elucidated; however possible candidates

might be insulin receptors (IRS)-1 and –2, which are associated with JAK1 and JAK3 and become

phosphorylated after IL-7 treatment. Both PI3K and IRS-1/2 are necessary for the proliferative

effects of IL-4 and IL-9 (Xiao et al., 2002).

An important key downstream target of PI3K, which had been shown in an IL-7- dependent mouse

thymocyte cell line (Li et al., 2004) and human thymocytes (Pallard et al., 1999), is the

serine/threonine kinase AKT. This critical component of the IL-2 family signaling (Kelly et al., 2002)

and probably the major effector of PI3K signaling, requires the c chain for activation (Jiang et al.,

2004). AKT is recruited upon phosphorylation and conversion of the lipid phosphatidylinositol-4,5-

bisphosphat (PIP)2 to PIP3 by PI3K (Vanhaesebroeck and Waterfield, 1999). AKT has about 900

cellular targets (Maddika et al., 2007) and is attributed to execute two major activities: metabolism

(which will be discussed in section I.2.5.3.) and regulation of cyclin-dependent kinases (CDKs),

which are required for cell cycle entry and downregulation of cell cycle inhibitors such as p27kip1

proliferation (Barata et al., 2001). AKT phosphorylates and thus inactivates Forkhead transcription

factors (Brunet et al., 1999) e.g. Foxp3, preventing the synthesis of the death proteins Bim and

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p27kip1

, which could be the trigger of apoptosis in primary human T cells (Stahl et al., 2002).

Another activity of AKT is the phosphorylation of the pro-apoptotic protein Bad, which results in its

inactivation by binding to 14-3-3 proteins (Datta et al., 2000). Thus, the PI3K/AKT pathway might

be a possibility to regulate Bad activity and consequently support pro T cell survival. However, it

has been shown that the inactivation of Bad by IL-7 only partially depends on the PI3K/AKT

pathway (Lali et al., 2004).

Furthermore, it is not sure whether the PI3K/AKT pathway is directly required for cell proliferation,

since it was found that IL-7 did not activate the PI3K pathway and phosphorylate AKT, although

cells were proliferating in presence of IL-7 (Lali et al., 2004; Osborne et al., 2007).

2.3.3. Ras/Raf/ERK pathway

Stimulation with IL-7 might also lead to activation of the p42/44 Extracellular-signal regulated

kinase (ERK) cascade, which regulates the activity of the pro-apoptotic protein Bim and the

sodium/hydrogen exchanger (NHE), leading to a neutral pH (discussed in section I.2.5.4.).

In T lineage but not B lineage cells, the induction of ERK appears to happen via the canonical

pathway involving Shc/Grb2/SOS. Alternatively, ERK activation may be linked to IL-7R signals via

Pyk2 (Benbernou et al., 2000), which becomes associated with JAK1 upon IL-7 stimulation.

However, according to Guinamard et al. (2000), this pathway might not be essential to connect the

IL-7R to the ERK pathway.

However, the ERK pathway is not induced in most cell types upon IL-7 stimulation, at least not in

murine T cell lines (Crawley et al., 1996; Kittiparin and Khaled, 2007). In contrast, it might be

induced in pre B cells (Fleming et al., 2001).

2.3.4. SFK pathway

Src family protein kinases (SFKs) are non-receptor tyrosine kinases, which are activated by IL-7

(Seckinger and Fourgereau, 1994), although none of the members yet have been shown to be

uniquely required for IL-7. SFKs include nine members, Src, Lck, Hck, Fyn, Blk, Lyn, Fgr, Yes and

Yrk, all with similar structure, but a unique sequence that confers specific functions.

Tyrosine phosphorylation of specific residues can increase or decrease the kinase activity of SFKs

and can thus be regulated by other kinases and phosphatases, such as CD45 (Huntington et al.,

2004). The two most abundantly expressed SFKs in T cells are Lck and Fyn (Mustelin, 1994).

Lck binds CD4 and CD8 co-receptor molecules and can interact with a variety of surface receptor

molecules including IL-7R (Isakov and Biesinger, 2000). It is uniquely required for thymocyte

development at the stage of pre-TCR signaling, which begins at the pro-T4 stage. In contrast, both

isoforms of Fyn, FynB (expressed in B cells) and FynT (expressed in T cells) are not uniquely

required for IL-7 receptor signaling in T cells (Lowell and Soriano, 1996). Upon IL-7 stimulation, Lck

and Fyn, which are associated with IL-7R in T lymphocytes, undergo phosphorylation (Page et al.,

1995).

In B cells the SFKs, Fyn and Lyn, are associated with the BCR and are involved in BCR-mediated

signaling; their activities are synergistic (Yasue et al., 1997).

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In conclusion, SFKs are activated by IL-7, but no single family member is essential. Thus, there

may be a requirement for redundant function from this family (Jiang et al., 2005).

2.4. IL-7 and cell cycle

IL-7 is not only important for survival of cells, but also for their proliferation. The different effects

can be distinguished from each other in cases where survival is induced without proliferation; this

occurs at low IL-7 doses (< 1ng/mL) (Li, 2004; Khaled and Durum unpublished, reviewed in Jiang

et al., 2005). However, it is still controversial whether IL-7 really works as a proliferative factor, as

oppositional results can be found in literature (Geiselhart et al., 2001; Rathmell et al., 2001; Munitic

et al., 2004; Beq et al., 2006). These disparate findings could be explained by the fact that

transcription and expression of the IL-7R is negatively regulated by its ligand, IL-7 (Park et al.,

2004; Munitic, 2004).

Although the pathway from IL-7R to cell cycle progression is still unknown, it is presumed that IL-7

regulates the transition from the G1 to the S phase (von Freeden-Jeffry et al., 1997). Important

factors for this transition are G1 cyclins and CDK2. Their activity is negatively regulated by p27kip1

,

which is a member of the CIP/KIP family of cyclin dependent cell cycle inhibitors (CKIs). For re-

activation of CDKs, the dephosphorylating activity of Cdc25A is required (Jinno et al., 1994). In

turn, Cdc25A is negatively regulated by phosphorylation, triggering its degradation through an

ubiquitin-proteasome dependent pathway (Bernardi et al., 2000). The phosphorylation of Cdc25A is

mainly induced by two kinase families: MAPK, specifically p38 MAPK (Khaled et al., 2005), and the

checkpoint kinases (CHKs) 1 and 2 (Goloudina et al., 2003). IL-7 withdrawal induces activation of

this stress kinase p38.

CDK2 may be an important downstream mediator in the IL-7 pathway, leading to proliferation.

Unlike in other growth factors however, the primary mechanism by which IL-7 induces proliferation

is supposed to be the regulation of the inhibitory factor p27kip1

and the CDK activator Cdc25a rather

than synthesis of cyclins (Jiang et al., 2005).

2.5. Lymphotrophic effects of IL-7

IL-7 is an obligate survival factor for several subsets of progenitor and mature lymphoid cells

(reviewed in Khaled, 2002, a). Deficiencies in IL-7 can lead to apoptosis in dependent cell lines

(von Freeden-Jeffry, 1997). Furthermore, IL-7 is required for homeostatic survival of peripheral T

lymphocytes (Tan et al., 2001), memory CD8 T cells (Schluns et al., 2000) and probably also CD4

cells (offset TCR engagement) (Seddon et al., 2003).

2.5.1. Induction of anti-apoptotic factors

One major factor of cell survival induction by IL-7 is the regulation of Bcl-2 family members. Bcl-2 is

a potent anti-apoptotic protein, which improves survival of T lymphocytes (Strasser et al., 1996),

but due to its anti-proliferative activity does not lead to an increase in T cells, as would a true

homeostatic regulator. However, Bcl-2 is not responsible for all IL-7 effects, as it cannot rescue

neither T cells (Nakajima and Leonard, 1999), nor B cells (Maraskovsky et al., 1998).

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Another anti-apoptotic protein of the Bcl-2 family is Bcl-XL. It is upregulated by IL-7 and rescues

primary T cells from death through IL-2 withdrawal (Amos et al., 1998). Above this, it is probably

one mediator of the PI3K pathway.

In addition to regulating Bcl-2 or Bcl-XL, IL-7 could also induce the expression of myeloid leukemia

cell differentiation protein (MCL)-1, another anti-apoptotic protein that could be responsible for

maintenance of IL-7 dependent lymphocytes, although MCL-1 induction in an IL-7-dependent

thymocyte line has not yet been observed (Opfermann et al., 2003).

2.5.2. Suppression of pro-apoptotic proteins

Aside from inducing anti-apoptotic factors, IL-7 also actively inhibits apoptosis by suppressing the

activity of pro-death proteins, which are also members of the Bcl-2 family. They are divided into two

groups: the „„multidomain‟‟ proteins, such as Bax and Bak, and the „„BH3‟‟ only proteins, such as

Bid, Bad and Bim. Upon posttranslational activation of these death proteins, their translocation to

mitochondrial membranes is initiated where they induce damage and release cytochrome c, which

in turn triggers the caspase cascade.

The „„BH3‟‟ only protein Bid binds to Bcl-2 or Bax and promotes cell death. Another „„BH3‟‟ only

protein, Bad, is phosphorylated by AKT after induction of the PI3K pathway (Franke et al., 1997).

Bad is a component of the death pathway inhibited by IL-7 and a potential apoptotic factor in T

lymphocyte development because T cells from Bad transgenic mice are highly sensitive to

apoptotic stimuli (Mok et al., 1999).

In contrast to the other two pro-apoptotic proteins already mentioned, Bim contains a hydrophobic

C-terminus in addition to the BH3 domain. It exists in three isoforms: BimS, BimL and BimEL

(O‟Connor et al., 1998). Upon apoptotic stimuli, Bim is released from the dynein motor complex by

a mechanism including phosphorylation on T56 and S58 by Jun N-terminal kinases (JNK), leading

to an increase in the apoptotic activity (Lei and Davis, 2003). Bim can be regulated by ERK, AKT,

STATs and the forkhead transcription factor, FKHR-L1. ERK reduces the apoptotic activity of Bim

and interaction with Bax by phosphorylating BimEL on three serine sites, S55, S65, and S100

(Harada et al., 2004). However as already mentioned, IL-7 treatment does not induce the ERK

pathway in most cell types. Bim plays a critical role in the cell death induced by IL-7 withdrawal

(Pellegrini et al., 2004); the relevant binding partner for Bim has been suggested to be the pro-

survival protein MCL-1, which can normally prevent the activation of Bax and Bak (Opfermann et

al., 2003).

Other pro-apoptotic proteins, which belong to the multidomain group of the Bcl-2 family having a

transmembrane domain, and which are potentially inhibited by IL-7, are Bak and Bax.

2.5.3. Regulation of metabolism: glucose

Garland and Halestrap recognized in 1997, that cytokines can upregulate glucose import and

metabolism. Thus, lacking of a cytokine signal can lead in cells depending on these cytokines to a

progressive atrophy and downregulation of glucose transporters such as GLUT1 (Summers and

Birnbaum, 1997) with an accompanying decreased activity of glycolytic enzymes (Plas et al., 2002)

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and loss of adenosine tri-phosphate (ATP) synthesis. As a consequence, cells decrease in cell size

or/and undergo apoptosis (Rathmell et al., 2000).

The downstream substrate of PI3K, AKT, seems to be important for glucose uptake, as forced

expression of AKT promoted transcription of GLUT1 (Bentley et al., 2003). Upon IL-7 withdrawal, a

loss of glucose uptake was rapidly observed, leading to the hypothesis, that T cells are dependent

on IL-7 for maintenance of metabolic activity (Rathmell et al., 2001). Since AKT is activated by IL-7,

it is likely that part of the survival signal through IL-7 also involves maintenance of glucose

metabolism.

Besides this, another nutrient transporter with high metabolic activity, the transferring receptor

(CD71), is regulated by IL-7. Its surface expression is equally blocked by PI3K inhibition.

2.5.4. Regulation of metabolism: pH

Cytokine deprivation leads to acidification in IL-7 dependent cell lines during the last steps of

apoptosis (Khaled et al., 1999). Reasons for this might be the breakdown of the pH regulatory

machinery or the release of protons from damaged mitochondria during apoptosis (Matsujama et

al., 2000). The acidic pH activates caspases and DNA nucleases and might also contribute to cell

death (Famulski et al., 1999).

Despite a metabolic activity, which generates acids, the intracellular pH of healthy growing cells is

neutral, through the action of several pH-regulatory proteins in the plasma membrane. One

example for these pH regulators in lymphocytes is the NHE, which exchanges excess intracellular

protons for extracellular sodium ions. The exchange activity of NHE can be increased by growth

factors via MAPKs. Likely pathways are MEK1, ERK and p90RSK, which phosphorylate NHE on

serine 703 in the intracellular, C-terminal domain (Takahashi et al., 1999). As a consequence, the

exchange function of NHE is increased and the acidic intracellular pH is raised up to a neutral

value. However, ERK is not activated by IL-7 (Crawley et al., 1996), although NHE is actively

phosphorylated in response to IL-7 signaling (Khaled et al., 2001). Thus another kinase increasing

NHE activity might be activated by IL-7.

In contrast to addition, withdrawal of cytokines leads to activation of stress MAPKs, e.g. p38 MAPK,

which phosphorylates NHE, leading to an alkalinization (up to levels over pH 7.5) (Khaled et al.,

1999). Due to this alkalinization, the death protein Bax translocates into mitochondria and thereby

blocks the import of adenosine di-phosphate (ADP), leading to a hyperpolarization of the

mitochondria. Consequently, ATP hydrolysis occurrs, which damages cells through the interruption

of the electron transport chain (ETC) and the subsequent generation of reactive oxygen species.

In summary, withdrawal of IL-7 creates via loss of glucose and cytosolic alkalinization severe

metabolic stress for dependent cell lines.

2.6. IL-7 in immunotherapy

Even if much progress has been made in the last years in immunotherapies to efficiently target

most cancers and infectious diseases, most of the therapies possess some disadvantages that limit

their full efficacy and development. The current limitations of most immunotherapies include e.g.

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insufficient production of T cells, as well as production of inefficient or short lived T cells, very

sensitive to apoptosis. Other problems are the fact that boosting CD4 counts but not CD8 counts,

or vice versa. Moreover it might happen that there is production of effector T cells with short lived

activity but not of central memory T cells that are responsible for long term protection, as well as

occasional production of more TH-2 or suppressor T-Regs than the required active TH-1 cells.

(Sportès and Gress, 2007; http://www.cytheris.com/ Science/interleukin7.php, 15.12.09).

Due to its multiple immune-enhancing properties, most notably in the maintenance of T cell

homeostasis, IL-7 is a very attractive candidate for immunotherapy in a wide variety of clinical

situations. In preclinical studies in murine and simian models, the efficacy of IL-7 has already been

shown. Thus, it was observed that cytotoxic T cells, which were adoptively transferred in vivo

protected mice against syngeneic tumors (Lynch et al., 1991; Jicha et al., 1991). IL-7 is now

emerging in human phase I trials as a very promising immunotherapeutic agent. The ability to

engraft human cells, both normal and neoplastic, into immunodeficient mice has allowed for the

examination of various potential biological therapies on human tumors in an in vivo setting (Mossier

et al., 1988; Rabinowich et al., 1992; Murphy et al., 1993, a). Moreover, the administration of rhIL-7

with adoptive immunotherapy (AIT) significantly prolonged the survival of human tumor-bearing

mice (Murphy et al., 1993, b). It can be assumed that IL-7 can resolve at least partly the above

mentioned limitations of current immunotherapies. This is achieved by systematically increasing the

number of CD4 and CD8 T cells in both animal models and in clinical studies, including simian

immunodeficiency virus (SIV) infected monkeys and human immunodeficiency virus (HIV) infected

patients (Sportès and Gress, 2007; Welch et al., 1989). Moreover, IL-7 administration is very potent

at producing “new long lived T cells” (i.e. naïve T cells and recent thymic emigrants) and to

augment lymphokine activated killer activity. It is particulary interesting, that IL-7 intervenes at all

stages of T cell development and maintenance. Moreover, it has been shown, that IL-7 in humans

induced a preferential expansion of naïve T cells, resulting in a broader T cell repertoire than

before the treatment; this effect was independent of age. This suggests that IL-7 therapy could

enhance immune responses in patients with limited naïve T cell numbers as in aged patients or

after disease-induced or iatrogenic T cell depletion (Nahed and Gress, 2010).

The two main immunological settings which correspond to various life threatening pathologies and

against which IL-7 could be used as an immunotherapeutic are CD4 T cell lymphopenia and the

case of inefficient specific immune response against massive antigen load such as that associated

with chronic viral infections, e.g. Hepatitis-C and HIV (http://www.glgroup.com/News/IL-7-

Immunotherapy-for-HIV-Pre-clinical-data-looks-promising-8486.html, 07.04.2010), as well as

different types of cancer (Goldrath, 2007; Sportès and Gress, 2007; http://www.cytheris.com/

Science/interleukin7.php, 15.12.09).

The Quality of IL-7 compounds can be monitored by biological assays, which will be thoroughly

discussed in the following section.

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3. QUALITY CONTROL OF BIOPHARMACEUTICALS

An important criterion in the development process of biopharmaceuticals is the monitoring of the

quality of the product. Quality control (QC) of biopharmaceuticals is achieved by using different

bioanalytical methods, amongst them biological assays, which are an indispensable method in this

context.

3.1. General remarks about quality control

Consumer and patient safety are the prerequisites for (bio)-pharmaceutical product development,

production and marketing. The ability to provide an effective, pure, safe product is the primary

factor determining the product‟s success (Doblhoff-Dier and Bliem, 1999). The quality of the

product thus needs to be controlled according to national and international guidelines. The major

factors under which the product is characterized are its purity, stability, safety and – last but not

least – its potency (International Conference on Harmonization (ICH) Q6B).

The successful development of novel pharmaceuticals cannot be achieved without the use of data

generated using validated bioanalytical methods (Nowatzke and Woolf, 2007). These bioanalytical

methods are based on a variety of physico-chemical and biological techniques such as

chromatography, immunoassay and mass spectrometry. One of the most important methods for

the QC of biopharmaceuticals are biological assays or bioassays, which measure the biological

activity of a product and are thus necesserary for a complete structural characterization of new

biological entities (NBEs). The development of new bioassay principles is a key requirement in the

QC field of biopharmaceuticals and is focus of this work.

Bioanalytical methods must be validated prior to and during use to engender confidence in the

results generated. According to the Food and Drug Administration (FDA), the fundamental criteria

for assessing the reliability and overall performance of a bioanalytical method are: the evaluation of

drug and analyte stability, selectivity, sensitivity, accuracy, precision, linearity and reproducibility.

The extent to which a method is validated is dependent on its prospective use, the number of

samples to be assayed and the use of the data (Buick et al., 1990).

3.2. Criterions for quality control of biopharmaceuticals

According to the ICH Q6B, biopharmaceuticals are characterized regarding the following aspects.

3.2.1. Physicochemical properties

In a physicochemical characterization, the composition, physical properties, and primary structure

of the desired product are determined. In addition, information regarding higher-order structure of

the desired product may be obtained by appropriate physicochemical methodologies.

Since biopharmaceuticals are at least partially produced by living organisms, an inherent degree of

structural heterogeneity can occur. Those post-translationally modified forms may be active and

harmless. Thus, if a consistent pattern of product heterogeneity is demonstrated, an evaluation of

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the activity, efficacy and safety (including immunogenicity) of individual forms may not be

necessary; however, lot-to-lot consistency has to be assured.

3.2.2. Biological activity

Since a complete structural characterization by physicochemical methods is – other than for small

molecules - not possible for biological products, bioassays are necessary for a full characterization

of a biological product to assess its biological activity. Bioassays with wider confidence limits may

be acceptable for QC of such products, when combined with a specific quantitative measure.

These methods asses the biological activity of a product, which is defined as the specific ability or

capacity of a product to achieve a defined biological effect. It can be measured using animal-based

assays, cell-based assays, biochemical assays or ligand and receptor binding assays (further

described in section 3.3.). The results of bioassays are potencies (expressed in units of activity) of

a sample in comparison to an adequate reference standard.

Potency is the quantitative measure of biological activity based on the attribute of the product which

is linked to the relevant biological properties. Mimicking the biological activity in the clinical situation

is not always necessary. A correlation between the expected clinical response and the activity in

the bioassay should be established in pharmacodynamic or clinical studies.

Since bioassays measure the potency of a product, they are also termed “potency assays”.

3.2.3. Immunochemical properties

In case of antibodies, a characterization of the immunological properties is necessary. Affinity,

avidity and immune-reactivity (including cross-reactivity) should be determined by using binding

assays of the antibody to purified antigens and defined regions of antigens. In addition, the target

molecule bearing the relevant epitope should be biochemically defined and the epitope itself

identified, when feasible.

In some cases, additional immunochemical analyses (e.g., enzyme-linked immuno sorbent assay

(ELISA) or western blotting), utilizing antibodies which recognize different epitopes of the protein

molecule, may be required to establish its identity, homogeneity or purity, or serve to quantify it.

3.2.4. Purity, impurities and contaminants

The purity of the drug substance and drug product is assessed by a combination of analytical

procedures, since the determination of absolute, as well as relative purity, presents considerable

analytical challenges, and the results are highly method-dependent. The purity is expressed in

terms of specific activity (units of biological activity per mg of product).

As a consequence of the unique biosynthetic production process, the drug substance can include

several molecular entities or variants. These molecular entities are part of the desired product,

when they are derived from anticipated post-translational modification. When they are formed

during the manufacturing process and/or storage and have properties comparable to the desired

product, they are considered product-related substances and not impurities.

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Impurities may be either process or product-related. Process-related impurities include those that

are derived from the manufacturing process, i.e. cell substrates (e.g. host cell proteins, host cell

DNA), cell culture (e.g. inducers, antibiotics, or media components), or downstream processing.

Product-related impurities (e.g. precursors, certain degradation products) are molecular variants

arising during manufacture and/or storage, which do not have properties comparable to those of

the desired product with respect to activity, efficacy, and safety. Impurities can be of known

structure, partially characterized, or unidentified. When adequate quantities of impurities can be

generated, these materials should be characterized to the extent possible and, where possible,

their biological activities should be evaluated. The acceptance criteria for impurities should be

based on data obtained from lots used in preclinical and clinical studies and manufacturing

consistency lots.

Contaminants in a product include all adventitiously introduced materials not intended to be part of

the manufacturing process, such as chemical and biochemical materials (e.g. microbial proteases),

and/or microbial species. Contaminants should be strictly avoided and/or suitably controlled with

appropriate in-process acceptance criteria or action limits for drug substance or drug product

specifications.

3.2.5. Quantity

Another critical aspect for a biotechnological and biological product is its quantity, usually

measured as protein content. The quantity determination is usually achieved in comparison to a

reference standard, but may also be independent of it. It is determined using an appropriate assay,

in most cases a physicochemical one. It is usual that the quantity values obtained may be directly

related to those found using the biological assay. When this correlation exists, it may be

appropriate to use measurement of quantity rather than the measurement of biological activity in

manufacturing processes, such as filling.

3.3. Biological assays

Biological assays, also termed bioassays or potency assays are an indispensable method for QC

of biopharmaceutical macromolecules, such as recombinant proteins or mononuclear antibodies.

3.3.1. Assay formats and requirements for use in QC

3.3.1.1. Overview of assay formats

There are various different assay formats used for QC of biopharmaceuticals. They reach from

immunoassays, such as ELISAs, over reporter gene assays, proliferation- and phosphorylation

assays to in vivo and in vitro disease assays. All of them possess their advantages and

disadvantages. In figure 3, an overview of the different assay formats is given, showing their clinical

relevance in comparison to their variability and thus suitability for QC.

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Increasing clinical relevance

In vivo disease animal model

In vivo animal assay

Cell based assay

primary cells

cell lines

Cell based biochemical assays

kinase receptoractivation

reporter gene

Binding assays

cell based receptorbinding

immunoassays

Physicochemical assays

Increasing variability

Decreasing suitability for QC

Figure 3. Overview of assay formats. Figure 3 gives an overview of the different assay formats. Assays with a high clinical relevance also show a high variability associated with a low suitability for QC and vice versa. Those parameters have to be balanced when choosing the right assay format. Source: Bachmann (2006)

The figure shows the correlation of clinical relevance versus variability, associated with the assays‟

suitability for QC. Physicochemical assays show a low variability and are thus well-suited for QC.

On the other hand, their clinical relevance lies not at hand. In contrast, in vivo disease assays are

of high clinical relevance, but also show a very high variability, which is problematic for QC

analysis. The two parameters clinical relevance and variability have thus to be balanced when

choosing the appropriate assay format.

3.3.1.2. Requirements for use in QC

As already described in section I.3.1., the successful development of novel pharmaceuticals cannot

be achieved without the use of data generated using well-functioning and validated bioanalytical

methods (Nowatzke and Woolf, 2007). All methods must be good manufacturing practice (GMP)-

conform as well as compliant with the criteria of the ICH guidelines and the guidances of the

authorities. In addition, the bioassays must be compliant with current statistical requirements of the

European Pharmacopeia (Ph.Eur.) and the United States Pharmacopeia (USP).

Assays used for quality control, release and stability testing should be precise, robust, accurate

and should show a good repeatability. To accomplish this and to be suitable for routine use in a QC

environment, they should provide a high signal to noise ratio and a stable read-out for more than

30min. Furthermore, they should be as fast as possible; kinetic measurements are usually not used

in QC.

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3.3.2. Analysis models for potency assays

The principle for the evaluation of potency assays is the comparison of a sample against a

reference standard on the basis of the measured biological activities (Ph. Eur. 6.7, 2010;

Gottschalk and Dunn, 2005, a). Due to the high variability of biologic systems, it is essential that

the tests on the standard and on the sample are carried out at the same time and under identical

conditions. Furthermore, randomization and independence of individual treatments are important

prerequisites to be considered (Ph. Eur. 6.7, 2010). After the performance of an assay and prior to

the calculation of the potency, an analysis of variance is carried out in order to check whether the

conditions of the different analysis models are fulfilled. Tests of significance of regression, linearity

(Hypothesis tests based on separate Analysis of Variance (ANOVAs)) and parallelism (Hypothesis

F-Test) are performed. As described in the Ph. Eur. 6.7, Chapter 5.3, a confidence interval of 99%

is used for the slope and a confidence interval of 95% is used for linearity and parallelism.

For evaluation of the potency, different statistical models are proposed e.g. the slope ratio assay,

comparison of EC50 values, the parallel line method and the logistic models four- and five-

parameter fit (Ph. Eur. 6.7, 2010; USP <111>, 2001; Wilbur, 1993). A good curve model should

accomplish three conditions: it must well approximate the true curve, needs to be capable of

averaging out as much of the random variation in the data as possible and should enable to predict

concentrations at points between the standard points and not only at the fitted data points

(Gottschalk and Dunn, 2005, b). Moreover, the model must be compliant with current statistical

requirements of the Ph.Eur. and the USP.

Some of the most commonly used calculation models to date are the parallel line method and the

logistic models four- and five-parameter fit, which will be presented in detail in the following.

3.3.2.1. The parallel line model

For dilution assays, usually several dose steps (e.g.

nine dilution steps, which is one commonly used

format at Merck Serono) are utilized, resulting in an

extended dose-response curve with a sigmoid shape.

Since such a high number of dose levels is not ethical

for some assay formats, e.g. in vivo assays or less

practical or since the aims of the assays might be

achieved with fewer dose responses, the dose

response range can be restricted to the linear range

of the curve. The restriction of the curve is for

example used by the parallel line (PL) assay, which

only utilizes the linear region of the sigmoid curve for

potency determinations, because this is the region of

the curve where the dose response is the steepest,

providing the best estimate of relative potency

(Finney, 1978; Bunch et al., 1990). The asymptotes are not taken into consideration (see figure 4).

Figure 4. Graphical presentation of the parallel line model.

Example of an assay with three dilution steps, analyzed by the PL model. Source: Ph. Eur. 6.7, chapter 5.3 (2010)

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Figure 5. Graphical presentation of the four-parameter fit. Example of an assay with 9 dilution steps, analyzed by the 4PL model. Source: Ph. Eur. 6.7, chapter 5.3 (2010)

The relationship between the dose X and the response Y is given by the following equation:

In which a is the intercept and b is the slope of the line.

Often, the dose must be log transformed to result in a straight line. Then, X equals log (dose).

Statistical validity on the following hypotheses can be tested:

1. The dose-response relationship is linear for the standard and the sample preparation.

2. The dose-response curve has a significant slope.

3. The dose-response curves of standard and sample preparation are parallel.

In comparison to the traditional single-point assay, the parallel line model has the advantage (by

checking the hypotheses mentioned above) that a linear dose-response correlation can be proven

and a dose-independent relative potency is obtained. The potency is defined as the distance

between the linear slope of the sample and the slope of the reference standard. Therefore, at least

three dilutions for both the test serial and the reference are required.

3.3.2.2. Logistic models (4-and 5-parameter fit)

In contrast to the PL model, the logistic models

consider the whole dose response range, resulting in

the advantage that additional information about the

asymptotes is given. This might lead to a higher

precision of the assay since the whole curve is

considered for potency determination. Disadvantages

in comparison to the PL model are the higher number

of dose levels required and the fact that these models

are currently less precisely described in the Ph. Eur.

The four-parameter fit (4PL) calculates a curve based

on four-parameters (Volund et al., 1978; Findlay and

Dillard, 2007): the response at infinite dose

(saturation), the response at minimal dose (extinction),

the 50% effective dose (ED50) and the slope of the

line (see figure 5).

This results in the following equation, describing the 4PL model:

in which Y is the response, D is the response at infinite analyte concentration, A is the response at

zero analyte concentration, X is the analyte concentration, C is the inflection point on the calibration

curve (IC 50 ), and B is a slope factor (Findlay et al., 2007).

Y = a + bX (Eq. 1)

Y = D + (A-D)/ [1+ (X/C)B]

(Eq. 2)

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By adding a fifth parameter, G, which controls the degree of asymmetry of the curve, the four-

parameter logistic model is expanded to the five-parameter fit (5PL) (Prentice et al., 1976; Straume

et al., 1994). With the extra flexibility afforded by its asymmetry parameter, the 5PL is able to

virtually eliminate the lack-of-fit error that occurs when the 4PL is fitted to asymmetric dose-

response data.

Consequently, it is advised to use the 5 PL model for calculation of asymmetric curves. The

equation for the 5PL model is the following:

The choice for the right model is a matter of frequent discussions and depends on the assay set

up. As a general rule, during validation of the assay it has to been shown that the assay including

the evaluation model chosen meets predefined acceptance criteria for e.g. accuracy and precision.

By this, the choice of the evaluation model can be justified.

3.3.3. Read-out system for proliferation assays

The most commonly assays used in QC of biopharmaceuticals are proliferation assays.

In the past, cell proliferation was mainly measured by using radioactive compounds, e.g. 51

Cr and

[3H]thymidine (Schlager and Adams, 1983) or tetrazolium salts like 3-(4,5-Dimethylthiazol-2-yl)-2,5-

diphenyltetrazoliumbromid (MTT) (Denizot and Lang, 1986; Hansen et al, 1989; Mosmann, 1983)

and sodium(2,3-bis(2-methoxy-4-nitro-5-sulfophenyl~-2H-tetrazolium-5-carboxanilide (XTT)

(Roehm, 1991). Although [3H]

thymidine is still used because of its high sensitivity, it is increasingly

replaced by more convenient, less harmful non-radioactive alternatives (Hamid, 2004; Rotter and

Oh, 1996). Three of the most commonly used reagents in this regard are the tetrazolium salt and

MTT analogue 3-(4,5-dimethylthiazol-2-yl)-5-(3-carboxymethoxyphenyl-2-(4-sulfophenyl)-2H-

tetrazolium) /phenazine methosulfate (MTS/PMS) (Goodwin et al., 1995), the fluorescent dye

Alamar Blue (Ahmed et al., 1994) and the ATP bioluminescence assay using the luciferase

reaction (Crouch et al., 1993; Kangas et al., 1984). The basic principles of these read-outs are

described in the following.

3.3.3.1. Colorimetric detection

The MTS/PMS assay is a colorimetric assay, which is based on the reduction of a tetrazolium salt

(MTS) to an intensely colored formazan by the mitochondria enzymes (dehydrogenases) of living

cells (Goodwin et al., 1995) (see figure 6). PMS acts as an intermediate electron acceptor and

accelerates the reaction. The amount of the produced formazan is directly proportional to the

number of living cells in culture and can be measured at 492nm (Malich et al., 1997).

In contrast to MTT, MTS/PMS has the advantage of being water-soluble. Thus, the solubilization

step of the crystals prior to measurement, which is required for MTT, can be eliminated. This

Y = D + (A-D)/ [1+ (X/C)B]G

(Eq. 3)

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I. INTRODUCTION

39

reduces both the risk of microbial contamination of the assay and the sample processing time

(Stevens and Olsen, 1993; Rotter and Oh, 1996).

Comparing the MTS substrate to another tetrazolium salt, XTT, Goodwin et al. (1995) discovered

that the XTT/PMS, but not the MTS/PMS, reagent mixture was unstable, which favors the use of

MTS instead of XTT. As a consequence, the MTS/PMS substrate was used as an example for the

colorimetric detection in this study, since it seemed to be the most advantageous of the three

tetrazolium salts.

Figure 6. Reaction equation of the colorimetric read-out. The basic principle of this reaction is the reduction of a tetrazolium salt into an intensely colored formazan, accelerated by the electron acceptor PMS. (NAD: Nicotinamid-adenin-dinucleotid, EC: ethylene carbonate)

3.3.3.2. Fluorescence

The fluorescent dye Alamar Blue has been proposed as a substitute for [3H]

thymidine (Ahmed et al.,

1994) and an alternative for the MTT assay (Pagé et al., 1993).

The native, oxidized state of Alamar Blue, resazurin, is non-fluorescent and blue. When

internalized by living cells, oxidoreductases and the mitochondrial electron transport chain reduce

this reagent intracellulary to resofurin, a highly fluorescent red dye (Goegan et al., 1995) (see figure

7). The amount of the fluorescence detected is proportional to the number of living cells.

The main advantage of this reagent is its low toxicity and its non-destructive effect on cells, in

contrast to most of the other reagents including MTS/PMS and the ATP bioluminescence assay.

These latter reagents induce cell death and consequently allow performing endpoint assays only,

whereas the use of Alamar Blue enables to carry out kinetic measurements of the changes in cell

proliferation, viability and metabolic activity (Pagé et al., 1993; Zhi-Jun et al., 1997). Moreover,

Hamid et al. (2004) found a higher sensitivity of the Alamar Blue assay in the detection of cytotoxic

effects compared with the MTT assay.

N

NN

N

NO2

SO3Na

SO3Na

I

N

NN

HN

NO2

SO3Na

SO3Na

I

EC-H EC

NAD+ NADH

RS

Tetrazolium salt (MTS)

Formazan

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I. INTRODUCTION

40

Figure 7. Reaction equation of the fluorescence read-out. The basic principle of this reaction is the reduction of the blue, non-fluorescent resazurin to the red fluorescent dye resofurin.

3.3.3.3. Luminescence

The ATP-bioluminescence assay measures the number of viable cells using the firefly luciferase-

luciferin system (Crouch et al., 1993) and can likewise be used as a read-out for proliferation

assays. Luciferase catalyzes the formation of light from ATP and luciferin in presence of Mg2+

ions

(see figure 8). The emitted light intensity is linearly related to the amount of ATP present and is

thus a direct measure of the number of viable cells (Andreotti et al., 1995; Mueller et al., 2004).

The ATP assay is supposed to be much more sensitive than the MTT assay and has slightly better

reproducibility (Petty et al., 1995; Weyermann et al., 2005). Disadvantages are the higher costs of

the luminescence reagent and the time-dependency (of some reagents) of the luminescence signal

(Weyermann et al., 2005).

Figure 8. Reaction equation of the luminescence read-out. The basic principle is the reaction from luciferin to oxyluciferin in presence of ATP and Mg

2+ions, catalyzed by

the enzyme luciferase.

3.4. Investigated biopharmaceuticals

The following biopharmaceuticals were used for the test of the different types of bioassays.

3.4.1. Cetuximab (Erbitux®)

Cetuximab is a recombinant, human/mouse chimeric monoclonal antibody that binds specifically to

the extracellular domain of the EGFR.

O

N

OOH

O

O

N

OOH

NADH/H+ NAD+, H2O

Resazurin Resofurin

N

SOH

S

N COOH

N

SOH

S

N OH

hv

Luciferase

Luciferin

ATP, Mg2+OxyluciferinAMP, CO2

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I. INTRODUCTION

41

EGFR is a major target of anti-cancer therapies, because its level of expression on tumor cells is a

hint regarding the aggressiveness of the tumor. Epidermal growth factors bind specifically on the

EGFR, inducing cell signaling cascades for cell proliferation. As a consequence, the tumor burden

increases and metastasizes. The anti-EGFR antibody blocks binding of growth factors to EGFR

specifically. Thus, proliferation and metastasis of cancer cells is blocked.

The investigated anti-EGFR antibody is composed of the Fv regions of a murine anti-EGFR

antibody with human IgG1 heavy and kappa light chain constant regions. It is produced in

mammalian (murine myeloma) cell culture and has a molecular weight of approx. 152kDa.

Therapeutic indications are colorectal cancer (CRC), squamous cell carcinoma of the head and

neck, non-small cell lung carcinoma (NSCLC), pancreatic cancer and renal cell carcinoma.

3.4.2. Tucotuzumab celmoleukin (KS-IL2)

Tucotuzumab celmoleukin is a genetically engineered fusion protein (immunocytokine), comprizing

a humanized monoclonal antibody directed against the Epithelial Cell Adhesion Molecule (EpCAM)

genetically fused to a human cytokine (IL-2). It is derived from an IgG1 mouse monoclonal antibody

reactive with the EpCAM antigen. EpCAM is one of the first tumor-associated antigens and is

expressed at high level and frequency on most human carcinomas; it is a prime target for

immunotherapies. Targeting of IL-2 to EpCAM-expressing tumors of epithelial origin produces a

multi-factorial immune response through antibody-dependent cellular cytotoxicity (ADCC) and

cytokine stimulatory effects in a wide range of tumor types. Apart from this antibody-dependent

effectors‟ mechanism, also a cytokine induced mechanism is induced due to the comprized IL-2

molecules. Thus, typical IL-2 responses are stimulated, such as inducing CTL and NK cells -

capable of recognizing and killing tumor cells.

Tumors that can be targeted with this molecule are most epithelial cancers, such as ovarian, small

cell lung carcinoma (SCLC), NSCLC, prostate, gastro-intestinal (GI) and breast cancer.

3.4.3. Fc-IL7

This cytokine fusion protein consists of the Fc domain of an antibody, linked to an IL-7 molecule.

IL-7 is a cytokine being important for the development of lymphocytes and T cells, which has

already been discussed thoroughly in the Introduction section. The Fc Domain, Fcγ2h, shows little

or no interaction with FcRs and leads to a significantly longer half-life than the pure IL-7; moreover,

it is more potent. It can thus be given less frequently.

It can be used against the following targeted indications:

Following autologous hematopoietic stem cell transplantation to reduce infection and

increase T cell response and survival;

Following standard chemotherapy regimens to increase anti-tumor response and survival;

In combination with tumor vaccine or adoptive T cell transfer in either of the above two

settings.

Furthermore, its applicability can be expanded against chronic or tropical disease including HIV,

malaria, dengue fever and auto-immune diseases.

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II. AIM OF THIS STUDY

42

IIII.. AAIIMM OOFF TTHHIISS SSTTUUDDYY

First aim of this study was the evaluation of optimized proliferation assays regarding different

analysis models and read-out systems newly established in the Merck Serono Bioassay

laboratory.

Concerning the analysis models, the parallel line model was compared to the logistic models, four-

and five-parameter fit. For this comparison, the different models were classified regarding

accuracy, precision and failure rate.

Regarding the read-out systems, the colorimetric read-out, using the MTS/PMS reagent, was

compared to luminescence and fluorescence techniques, using CellTiter- Glo®

and Alamar BlueTM

,

respectively. The parameters considered for this comparison were sensitivity - implying the needed

cell amount -, signal to noise ratios, incubation times, as well as accuracy and precision of the

different read-out systems.

Second aim of this study was to develop and qualify an additional, faster assay as an alternative to

the commonly used proliferation assays since those assays usually require several days of

incubation time with active pharmaceutical ingredient (API). One possibility for this purpose is the

use of phosphorylation assays, which can be completed much faster than the end-point

proliferation assays.

Development of the phosphorylation assay was done by using the example of Fc-IL7, a cytokine

fusion protein which contains IL-7. Consequently, it was the aim to screen the signaling pathways

of IL-7 by western blotting in order to identify a suitable target for development of a phosphorylation

assay. In parallel, the IL-7 and IL-2 signal transduction cascades were elucidated using western

blotting and flow cytometry since the signaling pathways of IL-7 belong to the less characterized

pathways in comparison to other cytokines.

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43

IIIIII.. MMAATTEERRIIAALLSS AANNDD MMEETTHHOODDSS

1. MATERIALS

1.1. Cell lines

Designation Description Cell type Culture

medium

Source

CTLL-2 Cytotoxic murine T lymphocytes,

dependent on IL-2

suspension RPMI 1640 ATCC

DiFi Human, Epidermal Growth Factor

receptor (EGFR)-positive carcinoma

cells

adherent DMEM/F12 ImClone

Kit 225 Human IL-2 dependent T

lymphocytes, proliferating also in

presence of IL-7

suspension RPMI 1640 EMD

Serono

PB-1 Murine IL-7 dependent pre-B cells suspension McCoy‟s 5A DSMZ

2E8 Murine IL-7 dependent B lymphocytes suspension IMDM +

Glutamax

ATCC

(ATCC: American Type Culture Collection; EMD: Emanuel Merck, Darmstadt; DSMZ: Deutsche Sammlung von Mikroorganismen und Zellkulturen)

In figure 9, microscopic images of the cell lines, used in this study, are shown.

PB-1 2E8 Kit 225

CTLL-2 DiFi

Figure 9. Microscopic images of the cell lines, used in this study.

Pictures were made in an amplification of 100x for PB-1, 2E8 and DiFi cells and an amplification of 200x for Kit 225 cells, by the laboratory of Dr. Christa Burger, Merck Serono, Darmstadt. The picture of the CTLL-2 cells is obtained from the ATCC at a scale bar of 100µm.

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44

1.2. Investigated biopharmaceuticals

In this study, different biopharmaceuticals were investigated, all from Merck Serono, Darmstadt.

1.2.1. Cetuximab (Erbitux®)

Cetuximab is a recombinant, human/mouse chimeric monoclonal antibody that binds specifically to

the extracellular domain of the EGFR. It is further described under I.3.4.1.

The quality of this product with regards to its potency can be controlled by using the DiFi potency

assay (described under III.2.4.1.2.).

1.2.2. Tucotuzumab celmoleukin (KS-IL2)

Tucotuzumab celmoleukin is an immunocytokine, comprizing a humanized monoclonal antibody

directed against the EpCAM genetically fused to a human cytokine (IL-2). It is further described

under I.3.4.2.

The quality of this product with regards to its potency can be controlled by using the CTLL-2

potency assay (described under III.2.4.1.1.).

1.2.3. Fc-IL7

This cytokine fusion protein consists of the Fc domain of an antibody, linked to an IL-7 molecule. It

is further described under I.3.4.3.

The quality of this product can be controlled by using the Kit 225 potency assay (described under

III.2.4.1.3.) or the STAT5 phosphorylation assay (described under III.2.5.).

1.3. Antibodies

1.3.1. Primary antibodies

Specificity Species/isotype Used

concentration

Application Company

AKT Rabbit IgG 1:1,000 WB CellSignalling

p-AKT (Ser473) Rabbit IgG 1:1,000 WB CellSignalling

Bcl-2 Rabbit IgG 1:1,000 WB CellSignalling

Bim Rabbit IgG 1:1,000 WB CellSignalling

p-Bim (Ser55) Rabbit IgG 1:1,000 WB CellSignalling

CD25 (human) Mouse IgG1 қ,

PE conjugated

20µg/mL FACS Becton Dickinson

CD25 (mouse) Rat IgG1 λ,

PE conjugated

20µg/mL FACS Becton Dickinson

CD122 (hu) Mouse IgG1 қ,

PE conjugated

20µg/mL FACS Becton Dickinson

CD122 (mu) Rat IgG2b қ,

PE conjugated

20µg/mL FACS Becton Dickinson

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45

CD127 (hu) Mouse IgG1 қ,

PE conjugated

20µg/mL FACS Becton Dickinson

CD127 (mu) Rat IgG2b қ,

PE conjugated

20µg/mL FACS Becton Dickinson

ERK Rabbit IgG 1:1,000 WB CellSignalling

p-ERK

(Thr202/ Tyr204)

Rabbit IgG 1:1,000 WB CellSignalling

Lck Rabbit IgG 1:1,000 WB CellSignalling

p-Lck (Tyr505) Rabbit IgG 1:1,000 WB CellSignalling

p38 MAPK Rabbit IgG 1:1,000 WB CellSignalling

p-p38 MAPK

(Thr180/Tyr182)

Rabbit IgG 1:1,000 WB CellSignalling

Pim-1 Mouse IgG 1:100 WB Santa Cruz

STAT1 Rabbit IgG 1:1,000 WB CellSignalling

p-STAT1 (Tyr701) Rabbit IgG 1:1,000 WB CellSignalling

STAT3 Rabbit IgG 1:1,000 WB CellSignalling

p-STAT3 (Tyr705) Rabbit IgG 1:1,000 WB CellSignalling

STAT5 Rabbit IgG 1:1,000 WB CellSignalling

p-STAT5 (Tyr694) Rabbit IgG 1:1,000 WB CellSignalling

STAT5 Rabbit IgG 1:100 ELISA CellSignalling

p-STAT5 (Tyr694) Mouse IgG 1:100 ELISA CellSignalling

(FACS: Fluorescence Activated Cell Sorting; WB: Western blotting; PE: Phycoerythrin)

1.3.1. Secondary antibodies

Specificity Species/isotype Used

concentration Application Company

Rabbit

Alexa Fluor 680

goat IgG 1:10,000 WB Invitrogen

Mouse

Alexa Fluor 680

goat IgG 1:10,000 WB Invitrogen

Rabbit HRP-linked IgG 1:1,000 ELISA CellSignalling

Rabbit HRP-linked IgG 1:2,500 ELISA Promega

(HRP: horseradish peroxidase)

1.4. Controls

1.4.1. Cell control extracts

Control Used for detection of Application Company

C6 glioma cells +

anisomycin

p-p38 MAPK WB CellSignalling

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46

CCRF-HSB-2 Lck, p-Lck WB Santa Cruz

Hela + IFN-α p-STAT5 WB CellSignalling

HT29 + IFN-α p-STAT1, p-STAT3 WB Inhouse

Hut 78 Bim, p-Bim WB Santa Cruz

Jurkat Bcl-2 WB Santa Cruz

Jurkat + Calycurin A p-AKT WB CellSignalling

K562 Pim-1 WB Santa Cruz

Kit 225 + FBS p-ERK WB Inhouse

Kit 225 + H2O2 p-p38 MAPK WB Inhouse

NIN/3T3 + heat shock p-p38 MAPK WB Santa Cruz

1.4.2. Isotype controls

Control Isotype Application Company

PE Mouse IgG1 қ

isotype control

Mouse (BALB/c) IgG1 қ FACS Becton Dickinson

PE Rat IgG1 қ isotype

control

Rat (LOU) IgG2b қ FACS Becton Dickinson

1.5. Culture medium, reagents and chemicals

Reagent Company

AIM-V medium Invitrogen

Alamar Blue™ Promega

Bovine serum albumin (BSA), Albumin fraction V Merck KGaA

β-mercaptoethanol (ME) Invitrogen

BME vitamins Promo Cell

Carbonate buffer Fluka Chemie

Cell Titer-Glo® Promega

Dimethyl sulfoxide (DMSO) Sigma

Dithiothreitol (DTT) Merck KGaA

DMEM/F12 medium Invitrogen

Dulbecco‟s phosphate buffered saline (DPBS)

without calcium and magnesium

PAA

Fetal bovine serum (FBS) Gibco or Invitrogen (for culture of 2E8 cells)

Glutamine Invitrogen

Glycine Merck KGaA

H2SO4 Merck KGaA

Hank‟s Buffered Salt Solution (HBSS) Sigma

HEPES Invitrogen

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47

Hu IL-2 Promo Kine (for culture of CTLL-2 cells) or

R&D Systems (for culture of Kit 225 cells)

Hu IL-7 R&D Systems

IMDM + Glutamax medium Invitrogen

McCoy‟s 5A medium Invitrogen

MEM essential amino acids Invitrogen

MEM non-essential amino acids Sigma

Methanol Merck KGaA

MTS/PMS cell proliferation reagent Promega

Mu IL-7 R&D Systems

NaCl Merck KGaA

Odyssey blocking buffer LI-COR

Orthovanadate Calbiochem

Roche complete mini-protease inhibitor cocktail Roche Diagnostics GmbH

RPMI 1640 medium Invitrogen

Sodium dodecyl sulfate (SDS) Merck KGaA

Sodium pyruvate Invitrogen

SeeBlue® Plus2 prestained standard (1x) Invitrogen

Tetramethyl benzidine (TMB) Moss Inc.

Tris-glycine-SDS running buffer (10x) Anamed Electrophorese GmbH

Tris-glycine-SDS sample buffer (2x) Anamed Electrophorese GmbH

Tris(hydroxymethyl)-aminoethan Merck KGaA

Triton X-100 Merck KGaA

Trypan blue solution Invitrogen

Trypsin Invitrogen

Tween 20 Merck KGaA

WP1066 Sigma

1.6. Composition of buffer & reagent solutions

FACS buffer DPBS + 5% FBS

Transfer buffer 48mM tris(hydroxymethyl)-aminoethan 39mM glycine 20% methanol 1.3mM SDS pH 9.2

Blocking buffer (WB) Odyssey blocking buffer / PBS 1:2

Blocking buffer (STAT5 assay) DPBS + 1% BSA (Albumin fraction V)

Incubation buffer (primary antibody) Odyssey blocking buffer / PBS (+ 0.2% Tween 20) 1:2

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48

Incubation buffer (secondary antibody) Odyssey blocking buffer / PBS (+ 0.2%

Tween 20 and 0.02% SDS) 1:2

Ponceau S solution 0.1g Ponceau S 5mL acetic acid 100% 95mL Milli Q water

Washing buffer (WB) DPBS + 0.1% Tween 20

Washing buffer (STAT5 assay) DPBS + 0.05% Tween 20

Lysis buffer 150mM NaCl 50mM HEPES 0.5% Triton X-100 2mM Orthovanadate 1x Roche complete mini-protease inhibitor cocktail in water

1.7. Equipment

Equipment Company

Balance MC210P Sartorius AG

EL808 Ultra Microplate Reader Bio-Tek

Centrifuge (MiniSpin) Eppendorf AG

Electrophoreses Blue Power 3000 Serva

Electrophoretic Transfer Kit 2117-250

NOVABLOT

LKB Bromma

FACScan™ flow cytometer Becton Dickinson

Focussing chamber Multiphor II Amersham Pharmacia Biotech

Focussing chamber XCell Sure Lock™ Invitrogen

Humidified CO2 cell culture incubator Kendro Laboratory products GmBH

Laminar flow biosafety cabinet Kojair Tech Oy

Magnetic stirrer IKA Werke GmbH & Co. KG

Megafuge 1.0 with rotor 2704 Kendro Laboratory products GmBH

Microscope DMIL Leica Microsystems GmbH

Neubauer hemocytometer and corresponding

coverslip

Marienfeld

Odyssey Infrared Imaging System LI-COR

pH meter Metrohm AG

Plate shaker Janke & Kunkel, IKA Werke GmbH & Co. KG

Power Supply Power Ease 500 Invitrogen

Synergy 2 Reader Bio-Tek

Water bath Gesellschaft für Labortechnik mbH

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1.8. Plastic ware and other materials

Materials Company

4-20% tris/glycine-gels Anamed Electrophorese GmbH

Cell culture flasks, 75 cm2 Falcon

Cell culture flasks, 25 cm2 Falcon

Cell culture plates, 96 well Greiner (suspension cells)

Cell culture plates, 96 well Falcon (adherent cells)

Chromatography paper 20x20cm Whatman

Black plates, 96 well Corning Costar

ELISA plates Nunc Brand, Thermo Fisher Scientific

FACS tubes Becton Dickinson

Falcon Blue Max Polypropylene coniconal tube

(15mL and 50mL)

Becton Dickinson

Multipipettes and corresponding sterile tips Eppendorf AG

Pipet boy accu IBS Integra Biosciences

PVDF membranes Millipore

Safe-lock tubes (0.5mL, 1.5mL, 2mL and 5mL) Eppendorf

Single (1-2500µL) and multi channel pipettes

and corresponding sterile tips

Eppendorf AG

Sterile pipettes for single use (5-50mL) Falcon

Sterile reagent reservoirs Corning Costar

White plates, 96 well Corning Costar

1.9. Software

Software Company

Cellquest Beckton Dickinson

Gen5 Bio-Tek

KC4 Bio-Tek

Odyssey 2.1 LI-COR

PLA 1.2 and 2.0 Stegmann Systems

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2. METHODS

2.1. Cell culture

2.1.1. CTLL-2 cells

CTLL-2 cells were cultured in RPMI 1640 medium containing 10% FBS and 80 U/mL IL-2 in a

density of 1x105 cells/mL (cultivation period of two days) or 3x10

4 cells/mL (cultivation period of

three days).

Flasks were incubated at 37°C, 5% CO2 and 95% relative humidity.

2.1.2. DiFi cells

DiFi cells were cultured in DMEM/F12 medium containing 10% FBS in a density of 1x106 cells/mL.

Flasks were incubated at 37°C, 7% CO2 and 95% relative humidity.

2.1.3. Kit 225 cells

Cells were cultured in RPMI 1640 medium containing 10% FBS and 45U/mL IL-2 in a density of

2.5x104 cells/mL.

Flasks were incubated at 37°C, 5% CO2 and 95% relative humidity.

2.1.4. PB-1 cells

Cells were cultured in McCoy‟s 5A medium supplemented with 15% FBS, 1mM sodium pyruvate,

2mM glutamine, 0.4% BME vitamins, 1xMEM non-essential amino acids, 0.5xMEM essential amino

acids, 50µM ME and 50ng/ml huIL-7 in a density of 1x106 cells/mL.

Flasks were incubated at 37°C, 5% CO2 and 95% relative humidity.

2.1.5. 2E8 cells

Cells were cultured in IMDM + Glutamax medium supplemented with 20% FBS, 50µM β-ME and

1ng/ml muIL-7 in a density of 5x105 cells/mL.

Flasks were incubated at 37°C, 7% CO2 and 95% relative humidity.

2.2. Determination of the cell density

The cell density of a suspension was determined by mixing approximately 50μl of the cell

suspension with an equal volume of trypan blue solution. The cells in the resulting suspension were

counted directly in a Neubauer chamber (volume: 0.1 µl/grid) using a microscope. Dead cells were

identified by cytoplasmic staining with trypan blue. A grid at the bottom of the chamber was used to

count the cells and the cell density (cells per mL) was calculated with the following formula:

Cellular density (cells/mL) = number of cells on the grid x dilution factor x104 mL

-1.

Adherent DiFi cells were trypsinized and washed with HBSS prior to determination of the cell

density.

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2.3. Thawing of cells

Cell aliquots were taken out of the liquid nitrogen tank and warmed immediately in a water bath to

37°C. Cells were transferred to a 15mL Falcon tube containing 9mL assay medium. Cells were

centrifuged and resuspended in assay medium. They were checked for their viability by trypan blue

stain. Cells were cultured in appropriate conditions and the following day, the cells were evaluated

for viability and density.

2.4. Potency assays (colorimetric proliferation assays)

2.4.1. Principles

2.4.1.1. CTLL-2 potency assay

The purpose of this test is to determine the biological activity (potency) of tucotuzumab celmoleukin

by a proliferation assay dependent on IL-2. The cells used for this bioassay (CTLL-2) are murine

CTLs; consequently, the assay is termed “CTLL-2 potency assay” in this study. CTLL-2 cells

depend on the growth factor IL-2 concerning proliferation and viability. The proliferation of the cells

is linear within a specific IL-2 concentration range.

According to the plate layout (see figure 10), both one dilution series of standard and sample is

pipetted in a 96 well plate. Afterwards the cells are seeded in the plate. Cell proliferation is

measured by means of tetrazolium salt MTS/PMS, which is reduced to the water soluble and

colored formazan by mitochondria enzymes (dehydrogenases) of living cells. After measuring the

absorption of the formazan photometrically, a dose response curve is plotted. As alternative to the

MTS/PMS reagent, luminescence and fluorescence read-outs are tested (see section IV.2.).

The activity of the sample is determined in comparison to the reference standard using the parallel-

line method, or the logistic models, four-and five-parameter fit (see section IV.1.).

2.4.1.2. DiFi potency assay

This test aims for determination of the potency of cetuximab. The chimeric, monoclonal anti-EGFR

antibody binds specifically to the EGFR and inhibits thus cell proliferation. The cells used for this

assay – DiFi cells - are human, EGFR positive carcinoma cells; consequently, the assay is termed

“DiFi potency assay” in this study.

The performance of the assay follows the same principle as described for the CTLL-2 potency

assay.

2.4.2.1. Kit 225 potency assay

The purpose of this test is to determine the potency of a Fc-IL7 by a proliferation assay dependent

on IL-7. The cells used for this bioassay (Kit 225 K6 T) are human T lymphocytes whose receptor

has a high affinity to IL-7; consequently, the assay is termed “Kit 225 potency assay” in this study.

The proliferation of the cells is linear within a specific concentration range.

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1 2 3 4 5 6 7 8 9 10 11 12

A Medium Medium Medium Medium Medium Medium Medium Medium Medium Medium Medium Medium

B Medium Cells + Std 1

Cells + Std 2

Cells + Std 3

Cells + Std 4

Cells + Std 5

Cells + Std 6

Cells + Std 7

Cells + Std 8

Cells + Std 9

Cells + Medium

Medium

C Medium Cells + Std 1

Cells + Std 2

Cells + Std 3

Cells + Std 4

Cells + Std 5

Cells + Std 6

Cells + Std 7

Cells + Std 8

Cells + Std 9

Cells + Medium

Medium

D Medium Cells + Std 1

Cells + Std 2

Cells + Std 3

Cells + Std 4

Cells + Std 5

Cells + Std 6

Cells + Std 7

Cells + Std 8

Cells + Std 9

Cells + Medium

Medium

E Medium Cells +

P 1 Cells +

P 2 Cells +

P 3 Cells +

P 4 Cells +

P 5 Cells +

P 6 Cells +

P 7 Cells +

P 8 Cells +

P 9 Cells + Medium

Medium

F Medium Cells +

P 1 Cells +

P 2 Cells +

P 3 Cells +

P 4 Cells +

P 5 Cells +

P 6 Cells +

P 7 Cells +

P 8 Cells +

P 9 Cells + Medium

Medium

G Medium Cells +

P 1 Cells +

P 2 Cells +

P 3 Cells +

P 4 Cells +

P 5 Cells +

P 6 Cells +

P 7 Cells +

P 8 Cells +

P 9 Cells + Medium

Medium

H Medium Medium Medium Medium Medium Medium Medium Medium Medium Medium Medium Medium

The performance of the assay follows the same principle as described for the CTLL-2 potency

assay.

Figure 10. General plate layout for potency assays. Figure 10 shows the general plate layout used in this study, which is one commonly used plate layout at Merck Serono for potency assays. In case of the DiFi assay, PBS is used instead of assay medium for the outer wells.

2.4.2. Protocols

2.4.2.1. CTLL-2 potency assay

The assay was performed using a solution of tucotuzumab celmoleukin. The antibody preparations

were diluted in RPMI 1640 medium to nine decreasing dilution steps. 100 L/well of this solution

was transferred to a 96 well plate (Greiner) in triplicates and mixed with an equal volume of cell

suspension that had been prewashed twice with HBSS and resuspended in assay medium to reach

a concentration of 5x105 cells/mL. The plate was incubated for 24 2 hours (h) at 37°C, 5% CO2

and 95% relative humidity. Then, 40 L/well of a MTS/PMS solution was added. Following another

incubation time of 2.5 – 3h, the absorbance was measured at 490nm (Bio-Tek EL808 Ultra

Microplate Reader) and the potency was calculated using the PLA software (PLA 2.0, Stegmann

Systems; settings see section III.2.4.3).

2.4.2.2. DiFi potency assay

DiFi cells were washed with HBSS and trypsinized. Cells were resuspended in DMEM/F12 medium

to reach a concentration of 1x105 cells/mL. 100 L of this cell suspension was transferred to the

inner wells of a 96 well plate (Falcon) and incubated for 15 5 minutes (min) at 37°C and 7% CO2.

11 L/well of a cetuximab‟s dilution in DPBS (1%, pH 7.2, sterile) was added at nine dilution steps

to a concentration range of 5 - 55nM. Each concentration was added in triplicates.

The plate was incubated for 96 2h at 37°C, 7% CO2 and 95% relative humidity.

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53

Then, 40 L/well of a MTS/PMS solution was added. Following another incubation time of 75

15min, the absorbance was measured at 490nm (Bio-Tek EL808 Ultra Microplate Reader). The

potency result was calculated using the PLA software (settings see section III.2.4.3).

2.4.2.3. Kit 225 potency assay

The assay was performed using the cytokine fusion protein Fc-IL7. The IL-7 preparations were

diluted in RPMI 1640 medium to nine decreasing dilution steps in a concentration range of 0.35-

40ng/mL. 70 L/well of this solution was transferred in triplicates to the corresponding inner well of a

96 well plate (Greiner) and mixed with an equal volume of starved cell suspension (3 days

starvation in AIM-V medium) that had been prewashed twice with HBSS and resuspended in assay

medium to reach a concentration of 1.43x106 cells/mL (1x10

5 cells/well).

The plate was incubated for 96 2h at 37°C, 5% CO2 and 95% relative humidity.

Then, 40 L/well of a MTS/PMS solution (Promega) was added. Following another incubation time

of 3 – 4h, the absorbance was measured at 490nm (Bio-Tek EL808 Ultra Microplate Reader). The

potency result was calculated using the PLA software (settings see section III.2.4.3).

2.4.3. Data evaluation: comparison of different analysis models

For comparison of the different analysis models (see section IV.1.), the CTLL-2 and DiFi assays

were performed using three different concentration ranges.

The first one was optimized for the parallel line model (A: CTLL-2: 5-30ng/mL, DiFi: 2-12nM), the

second one adapted to the logistic models (B: CTLL-2: 0.75-100ng/mL, DiFi 0.25-95nM) and the

third one was in between the other two ranges and had been used in a validated potency assay

before (C: CTLL-2: 6.8-80ng/mL, DiFi: 5-55nM).

For both assay systems, six repetitions were performed for each sample concentration of 50%,

100% and 150% in comparison to the 100% standard. The percentages were based on the original

sample concentrations, e.g. 100% equals a dose range of 5 - 30ng/mL, 50% equals a dose range

of 2.5 – 15ng/mL and 150% equals a dose range of 7.5 – 45ng/mL. The experiments were

performed independently on different days. Experiments with concentration ranges (B) and (C)

were analyzed using PL, 4PL and 5PL; experiments with the closer concentration range (A) only

using PL. The selected ranges for calculation of the potencies in the PLA software were “best

range” for PL analysis (automatic detection individual range; minimal number of points: three) and

“full range” for 4 and 5PL analyses. Results were expressed as potency of the sample relative to

the reference standard.

For evaluation of the data, tests of significance of regression, linearity (Hypothesis tests based on

separate Analysis of Variance (ANOVAs)) and parallelism (Hypothesis F-Test for significant

deviations from parallelism) were used. The confidence interval was 99% for the slope and 95% for

linearity and parallelism according to the guidelines of Ph. Eur. 6.7, Chapter 5.3. No outlier tests

were performed.

Mean values, as well as standard deviations (SD [%]), coefficients of variation (CV [%]) and mean

relative errors (RE [%]; definition: mean value of the difference between the measured and the

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54

expected activity, divided by the expected activity) were calculated, in order to compare accuracy

and precision of the different models. For the purpose of testing a significant difference between

the models, a statistical analysis was performed by Enrico Tucci (National Institute of Statistics,

Rome, Italy; used software: Statgraphics, Warrenton, VA; see Appendix). For statistical evaluation,

the recovery was used instead of the calculated potency result since the data referred to different

concentration levels (50%, 100%, 150%). In order to check whether the data could be adequately

modeled by a normal distribution, the Kolmogorov-Smirnov (KS) test was used. If this was the

case, the Cochran‟s (C) test was applied for variance check of the SDs. Otherwise, the Levene‟s

(L) test was used. In cases where standard deviations were not significantly different, an ANOVA

test was performed on the mean values. In other cases, a Kruskal-Wallis (KW) test was applied on

the medians instead of the mean values.

The failure rate consists of the ratio of failed assays to all assays performed in percent. Failed

assays were defined as assays which failed due to linearity and similarity failure of the PLA test

based on preset acceptance criteria (99% confidence interval for the slope and 95% for linearity

and parallelism). For comparison of the failure rates, the hypothesis was made, that the failure rate

was the same for all three models and was equal to the mean value. The mean value was then

compared to the individual failure rates. A p-value < 0.05 indicated a statistically significant

difference.

Furthermore, it was investigated whether it was necessary to use “weighted” regressions.This is

the case, if the SDs of the different dilution points are not constant over the concentration range.

For application of “weights”, different transformations exist, e.g. reciprocal, log or square root

transformations. In this study, calculations according to DeSilva et al. (2003) and the USP <111>

(2001) were done, in order to find out whether the weighting procedure was necessary. According

to DeSilva et al. (2003), weighting is appropriate, if a plot of the pooled SDs versus the mean

responses reveals a linearly increasing relationship on a logarithmic scale. According to the USP,

weighting is recommended, when the plot of the sample variance is proportionally increasing to a

function of dose, e.g. dose squared. If the data follow a horizontal line, no weighting is needed.

2.4.4. Adaption of assay parameters to luminescence and fluorescence techniques

For comparison of the different read-out systems (see section IV.2.), the following parameters had

to be modified when using CellTiter- Glo® or Alamar Blue™ instead of MTS/PMS for all three

potency assays, CTLL-2, DiFi and Kit 225: concentration ranges, volume of substrates, APIs and

cells, incubation times with substrate and cell densities.

Modifications were considered successful if the signal to noise ratio could be increased.

Exact parameters developed for each assay system are shown in the results section.

For luminescence measurements, white plates, for fluorescence measurements, black plates were

used. Plates were measured in the Synergy 2 Reader (Bio-Tek) (wavelengths for fluorescence: Ex

= 530nm; Em = 600nm; 50% mirror). Potency results were determined using the PLA software.

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2.5. STAT5 phosphorylation assay

2.5.1. Principle

When IL-7 binds to the IL-7R on Kit225 cells, a signal transduction cascade is initiated, leading to

the phosphorylation of STAT5. The amount of phosphorylated STAT5 can be measured using this

ELISA based assay: If phospho-STAT5 is in the sample, it binds to the ELISA plate, coated over

night with anti-phospho-STAT5 antibody. After immobilization of the antigen (STAT5), the anti-

STAT5 detection antibody is added, forming a complex with the antigen. Between each step, the

plate is washed with a mild detergent solution to remove any particles that are not specifically

bound. The detection antibody is detected by a secondary HRP-conjugated antibody. HRP is an

enzyme, which catalyzes the conversion of the substrate TMB to a colored product, whose

absorption can be measured at 450nm.

2.5.2. Protocol

The assay was performed using two separate microtiter plates: the first one for cell stimulation and

lysis, the second one for ELISA.

The ELISA plate was coated over night with anti-phospho-STAT5 capture antibody (1:100 in 50mM

carbonate buffer, pH 9.6, 100µL/well) at 4°C and blocked the next day with 1% BSA (Albumin

fraction V) in DPBS for approx. 90min with gentle agitation at approx. 300 rounds per minute (rpm).

Kit 225 cells were starved 1 day without growth factor in a density of 5x105 cells/mL. The next day,

cells were washed twice with HBSS and resuspended in AIM-V medium to reach a concentration of

7.15x105 cells/mL (5x105 cells/well). 70 L of this cell suspension was transferred to the inner wells

of a 96 well plate (Greiner). 10 L/well of Fc-IL7 was added at nine dilution steps to a concentration

range of 0.4 – 100ng/mL. Each concentration was added in triplicates.

The plate was incubated for 10-15min at 37°C, 5% CO2 and 95% relative humidity.

20µL of 5 fold concentrated lysis buffer [750mM NaCl, 250mM HEPES, 2.5% Triton X-100, 10mM

Orthovanadate, 5x Roche complete mini-protease inhibitor cocktail in water] was added directly

(without centrifugation) to each inner well of the 96 well plate. The plate was agitated with 300rpm

on a plate shaker for 60min at RT.

Then, the cell lysates were transferred to the blocked ELISA plate (85µL/well) and incubated for

60min at room temperature (RT) under agitation. The plate was washed three times (DPBS +

0.05% Tween 20) and incubated with anti-STAT5 detection antibody (1:100 in blocking buffer,

100µL/well) over night at 4°C. The free antibody was washed away and 100µL/well HRP-

conjugated anti-rabbit antibody (1:2,500 in blocking buffer) was added. The plate was agitated

gently (300rpm) on a plate shaker for 60min at RT.

After washing, 100µL TMB was added to each well. The reaction was allowed to proceed for 20min

and then stopped with 100µL/well 1N H2SO4.

The absorbance was measured at 450nm (Bio-Tek EL808 Ultra Microplate Reader) and the

potency result was calculated using the parallel line method (PLA 2.0, Stegmann Systems).

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56

During assay optimization, different parameters were varied. For this, experiments were run in

triplicates to confirm the results. A high opticale density (OD) difference between 100ng/mL IL-7

and the control (0ng/mL IL-7) was used as a quality criterion in order to find the best conditions.

After assay optimization, the assay was qualified with respect to accuracy and precision. Therefore,

three repetitions were performed on three different sample concentrations of 50%, 100% and 150%

in comparison to the 100% standard (n = 9). The assays were performed independently on

different days.

REs as well as SDs and CVs were calculated, in order to evaluate accuracy and precision of the

assay.

2.6. Western blotting analysis

2.5.1. Principle

Immunoblotting or western blotting is used to identify specific antigens recognized by polyclonal or

monoclonal antibodies. In this study, Western blotting was used to identify targets which are up- or

downregulated by stimulation with IL-7 and which could consequently be used as targets for a

suitable bioassay.

Following solubilization with SDS and DTT, the proteins are separated by SDS-Polyacrylamide

gelelectrophoresis (SDS-PAGE) and the antigens are electrophoretically transferred to a

polyvinylidenfluorid (PVDF) membrane, a process that can be monitored by reversible staining with

Ponceau S. The transferred proteins are bound to the surface of the membrane, providing access

to immune-detection reagents. After non-specific binding sites are blocked by immersing the

membrane in a solution containing a protein or detergent blocking agent, the membrane is probed

with the primary antibody and washed. The antibody-antigen complexes are identified with a

secondary Alexa Fluor 680 anti-IgG antibody and detected using infrared (IR) fluorescence.

2.5.2. Protocol

Cells were starved in culture medium without growth factor for 1 day prior to incubation with IL-7 or

IL-2. The stimulation experiment was carried out with 100ng/mL IL-7 or IL-2 for various times at

37°C. After centrifugation, cells were solubilized with 100µL lysis buffer [150mM NaCl, 50mM

HEPES, 0.5% Triton X-100, 2mM Orthovanadate, 1x Roche complete mini-protease inhibitor

cocktail in water] and incubated for 1h at RT with gentle agitation. The lysates were centrifuged for

5min at 1100rpm to remove cell debris.

Cell lysates were subjected to SDS-PAGE using 4-20% tris/glycine-gels. Due to different protein

contents of the cells and to achieve a homogenous loading of the gel with equal protein amounts

for each cell line, the following cell numbers were used per lane: Kit 225: 3.5x104 cells/ lane, PB-1:

2.8x105 cells/ lane and 2E8: 2.5x10

5 cells/ lane. The separated proteins were electrotransferred to

a PVDF membrane in transfer buffer (48mM TrisBase, 39mM glycine, 20% methanol, 1.3mM SDS;

pH 9.2). Equivalent loading of the gel was checked by Ponceau S staining. The membrane was

incubated with Odyssey blocking buffer / PBS 1:2 for 1h and then incubated with different

antibodies (see section 1.3) over night at 4°C. The secondary Alexa Fluor 680 antibody was

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57

applied for 1h at RT in the dark. The blots were detected using IR fluorescence, Odyssey Infrared

Imaging System (LI-COR).

2.7. Inhibition with WP1066

2.7.1. Principle

(E)-3(6-bromopyridin-2-yl)-2-cyano-N-((S0-1-phenylethyl)acrylamide), WP1066, is a novel, more

potent AG490 analogue (Iwamaru, 2007). It is supposed to inhibite JAK2 and its downstream STAT

and PI3K pathways (Ferrajoli, 2007).

Incubation of a sample with WP1066 prior to stimulation with IL-2 or IL-7 was used to investigate

whether the signaling pathway was blocked by WP1066.

2.7.2. Protocol

WP1066 was dissolved in DMSO. A stock solution was made at a concentration of 10mM in DMSO

and stored at –20°C.

Prior to stimulation with IL-2 or IL-7, cells were incubated with 10µM WP1066 for 24h. Cells were

then incubated with IL-2 or IL-7 for 10min at 37°C and subjected to western blotting analysis as

described previously.

2.8. Flow cytometric analysis

2.8.1. Principle

Flow cytometry is a technique for counting and examing microscopic particles, such as cells.

Particles are hydrodynamically-focused and pass a beam of light. As a consequence, they scatter

light and fluorochromes are excited to a higher energy state. This combination of scattered and

fluorescent light is picked up by the detectors, and, by analyzing fluctuations in brightness at each

detector, it is then possible to derive various types of information about the physical and chemical

structure of each individual particle.

A specialized type of flow cytometry is FACS: Cells are incubated with fluorescence-labeled

antibodies, directed against specific surface antigens on the cells (e.g. CD127 = IL-7R) and then

sorted according to these attributes.

2.8.2. Protocol

For preparation of the flow cytometric analysis, 2 - 3x105 cells, which had been starved 24h without

growth factor, were centrifuged and washed twice with 4mL DPBS supplemented with 5% FBS.

Cells were then either labeled with isotype controls (PE mouse IgG1 қ or PE rat IgG2b қ isotype

controls) or PE-conjugated CD25 (detection of IL-2Rα), CD122 (detection of IL-2Rβ) or CD127

(detection of IL-7Rα). After 30min incubation on ice, cells were washed again and resuspended in

250µL DPBS + 5% FBS.

Cells were analyzed with a FACScan flow cytometer using Cellquest software (Becton Dickinson).

10,000 cells were analyzed from each sample. Cell debris and clumps were excluded by setting a

gate on forward scatter versus side scatter.

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IIVV.. RREESSUULLTTSS AANNDD DDIISSCCUUSSSSIIOONN

1. COMPARISON OF DIFFERENT ANALYSIS MODELS (PARALLEL LINE, 4-AND 5-PARAMETER FIT)

FOR POTENCY ASSAYS

For evaluation of the potency of a biological sample in comparison to a reference standard,

different statistical models are proposed (see Introduction, section I.3.3.2.). The most commonly

used calculation models to date are the parallel line method and the logistic models four- and five-

parameter fit. The PL model only utilizes the linear range of the curve for potency determination,

whereas the logistic models consider the whole dose response range including the lower and the

upper asymptote of the curve. The difference between the 4PL and 5PL model consists of an

additional fifth asymmetry parameter for the latter model.

In this study, the three analysis models for potency assays were compared to each other regarding

their suitability for QC purposes by means of the parameters accuracy, precision and failure rate.

This was done by using two different bioassay systems, the CTLL-2 and DiFi potency assays, and

three different sample concentrations of 50%, 100% and 150% in comparison to the reference

standard. The analysis models were compared to each other within the same software. The PLA

software from Stegmann Systems (Rodgau, Germany) was selected, which is an accepted and

widely used software in the QC analysis field for potency assays.

1.1. CTLL-2 potency assay

1.1.1. Concentration ranges

The CTLL-2 potency assay measures the IL-2 activity of immunocytokines by cell proliferation of

IL-2 dependent cells.

The assay was performed as described under Materials and Methods. In order to be able to

compare the different models, first of all, adequate concentration ranges and curves for the PL

model and the logistic models were developed using the original assay (concentration range C) as

a basis. The assay was performed on three different concentration ranges: the first one was

optimized for the PL model (A: 5-30ng/mL, see figure 11A) with the aim to have as many points as

possible in the linear range of the curve, the second one adapted to the logistic models (B: 0.75-

100ng/mL, see figure 11B) with the aim to have three points each in the minimal, linear and

maximal range of the curve and the third one was in between the other two ranges and had been

used in a validated potency assay before (C: 6.8-80ng/mL, see figure 11C).

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Standard Curve

0

0,2

0,4

0,6

0,8

1

1,2

1 10 100

x

y

Concentration [ng/mL]

OD

valu

es

at

490

nm

A

Standard Curve

0

0,2

0,4

0,6

0,8

1

1,2

0,1 1 10 100 1000

x

y

OD

va

lue

s a

t 4

90

nm

B

Concentration [ng/mL]

Standard Curve

0

0,2

0,4

0,6

0,8

1

1,2

1 10 100

x

y

Concentration [ng/mL]

OD

va

lues a

t 4

90

nm

C

Figure 11. Concentration ranges of the CTLL-2 potency assay. The assay was performed on three different concentration ranges convenient for the different analysis models. The resulting, representative curves are shown: a close range (A: 5-30ng/mL, see figure 11A), a wide range (B: 0.75-100ng/mL, see figure 11B) and an intermediate range (C: 6.8-80ng/mL, see figure 11C). Green points indicate the individual results, red points the mean values of the triplicates.

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1.1.2. Test on the necessity of “weighting”

It is frequently discussed in literature that it might be appropriate to use “weighted” regressions if

variance homogeneity of the data is not given (USP <111>,2001; Ph. Eur., 2010; DeSilva et al.,

2003). This is the case, if the SDs of the different dilution points are not constant over the

concentration range. This characteristic is termed “heteroscedasticity” (Findlay and Dillard, 2007).

Often, SDs are higher at increasing concentrations. This leads to a domination of the high

responses over the low responses. In order to avoid this, weighted regressions are used, which

place less “weight” on responses that exhibit higher variation and guarantee that all dilution points

contribute equally. Weighting might lead to a broader assay range and more accurate and precise

results. For application of “weights”, different transformations exist, e.g. reciprocal, log or square

root transformations. The right transformation is dependent on different factors and has to be

determined individually for each concentration point prior to the weighting procedure.

In literature, different criteria for tests on the necessity of weighting can be found. According to

DeSilva et al. (2003), weighting is appropriate, if a plot of the pooled SDs versus the mean

responses reveals a linearly increasing relationship on a logarithmic scale. According to the USP,

weighting is recommended, when the plot of the sample variance is proportionally increasing to a

function of dose, e.g. dose squared. If the data follow a horizontal line, no weighting is needed.

In this study, the calculations were made according to both, DeSilva et al. and the USP and the

results from these calculations are shown in figures 12 and 13.

When the pooled SDs were plotted against the mean absorbance (according to DeSilva et al.; see

figure 12), a slight trend to increasing SDs at increasing responses could be noted in some of our

curves. However, there was no linearly related relationship between them and the slope was < 1 in

all cases. In most cases, SDs increased first and than remained constant or even decreased again.

A

CTLL-2 assay: concentration range 5 - 30ng/mL

y = 0,6635x - 1,9713

R2 = 0,8199

-2,5

-2

-1,5

-1

-0,5

0

0 0,2 0,4 0,6 0,8 1

absorbance

log

[s

tan

da

rd d

ev

iati

on

]

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61

B

CTLL-2 assay: concentration range 0.75 - 100ng/mL

y = 0,7018x - 1,9726

R2 = 0,7456

-2,5

-2

-1,5

-1

-0,5

0

0 0,2 0,4 0,6 0,8 1

absorbance

log

[sta

nd

ard

devia

tio

n]

C

CTLL-2 assay: concentration range 0.75 - 100ng/mL

y = 0,7018x - 1,9726

R2 = 0,7456

-2,5

-2

-1,5

-1

-0,5

0

0 0,2 0,4 0,6 0,8 1

absorbance

log

[sta

nd

ard

devia

tio

n]

Figure 12. Plot of the pooled standard deviations (n = 18) vs. the measured mean responses for each concentration point. Illustrations are given for the different concentration ranges of the CTLL-2 potency assay (fig. 12A: 5-30ng/mL; fig. 12B: 0.75–100ng/mL; fig. 12C: 6.8-80ng/mL). According to DeSilva (2003), weighting is appropriate, if a plot of the pooled standard deviations vs. the mean responses reveals a linearly increasing relationship on a logarithmic scale.

When the pooled SDs were plotted against dose squared (according to the USP; see figure 13), no

increase at increasing concentrations could be noticed. The data followed approximately a straight

line.

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A

CTLL-2 assay: concentration range 5 - 30ng/mL

y = 0,0003x - 1,6192

R2 = 0,3591

-2,5

-2

-1,5

-1

-0,5

0

0 200 400 600 800 1000

dose squared

log

[s

tan

da

rd d

ev

iati

on

]

B

CTLL-2 assay: concentration range 0.75 - 100ng/mL

y = 3E-05x - 1,6148

R2 = 0,1623

-2,5

-2

-1,5

-1

-0,5

0

0 2000 4000 6000 8000 10000 12000

dose squared

log

[sta

nd

ard

devia

tio

n]

C

CTLL-2 assay: concentration range 6.8 - 80ng/mL

y = 2E-05x - 1,4535

R2 = 0,1152

-2,5

-2

-1,5

-1

-0,5

0

0 1000 2000 3000 4000 5000 6000 7000

dose squared

log

[sta

nd

ard

devia

tio

n]

Figure 13. Plot of the pooled standard deviations (n = 18) vs. the dose squared for each concentration point. Illustrations are given for the different concentration ranges of the CTLL-2 potency assay (fig. 13A: 5-30ng/mL; fig. 13B: 0.75–100ng/mL; fig. 13C: 6.8-80ng/mL). According to the USP, weighting is recommended, when the plot of the sample variance is proportionally increasing to a function of dose, e.g. dose squared. If the data follow a horizontal line, no weighting is needed.

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A B CA B C

It might be discussed whether weighting in case of this study would be appropriate according to the

calculations proposed by DeSilva et al.; in any case, it was not necessary according to the

calculations made according to the USP, the regulatory guideline.

As a consequence, unweighted regressions were used in this study for all concentration ranges of

the CTLL-2 potency assay.

1.1.3. Results

For the CTLL-2 potency assay, six repetitions were performed for each sample concentration of

50%, 100% and 150% (0.5, 1 and 1.5 relative potency) in comparison to the 100% standard,

independently on different days. Experiments with concentration ranges (B) and (C) were analyzed

using PL, 4PL and 5PL, experiments with the closer concentration range (A) only using PL. Mean

values, as well as SDs, CVs and REs were calculated, in order to compare accuracy and precision

of the different models. For the purpose of investigating the difference between the models, a

statistical analysis was performed by Enrico Tucci (Statgraphics, Warrenton, VA; see Appendix;

further described under Materials and Methods). Furthermore, the failure rates of the different

models were compared to each other. Failed assays were defined as assays which failed due to

linearity and similarity failure of the PLA test based on preset acceptance criteria (see sections

I.3.3.2. and II.2.4.3.).

Results of the CTLL-2 potency assay for the PL model, 4PL model and 5PL model varied between

75.3% and 147.4% recovery, 84.8% and 140.0% recovery and 84.2% and 137.6% recovery,

respectively. A mean accuracy (including all results) of 104.0% (recovery) 11.8% (mean RE) was

calculated for the PL model, whereas accuracies of 102.4% 8.5% and 102.3% 8.5% were

assessed for the 4PL and 5PL model, respectively. As an example, individual, representative

graphs are shown in figure 14.

Figure 14. Individual, representative graphs (calculated by PLA) of a CTLL-2 potency assay. Results of an assay with a target concentration of 150%, analyzed by the PL model (see figure 14A), the 4PL model (see figure 14B) and the 5PL model (see figure 14C) are shown.

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Results with an expected activity of 50% varied between 98.0% and 116.0% recovery with REs

between 7.5% and 21.8% and CVs between 9.3% and 21.7%. They are shown in table 3 and figure

15.

Table 3. Results CTLL-2 potency assay: expected activity 50% (i.e. relative potency: 0.5).

Figure 15. Results CTLL-2 potency assay: expected activity 50%. Mean values of six repetitions are shown for each concentration range and analysis model. Error bars indicate the mean CVs. The red, dashed line demonstrates the expected activity of 50%.

-

PL

(5-

30ng/

mL)

PL

(0.75-

100ng/

mL)

4PL

(0.75-

100ng/mL)

5PL

(0.75-

100ng/mL)

PL

(6.8-

80ng/mL)

4PL

(6.8-

80ng/mL)

5PL

(6.8-

80ng/mL)

Result assay 1 0.597 0.466 failed failed 0.737 0.7 0.688

Result assay 2 0.733 0.431 0.47 0.487 0.417 failed failed

Result assay 3 0.514 0.575 0.57 0.579 0.619 failed failed

Result assay 4 0.500 0.468 0.46 0.462 0.559 0.557 0.561

Result assay 5 0.509 0.508 0.54 0.539 0.585 0.585 0.581

Result assay 6 0.626 0.492 0.51 failed 0.429 0.443 0.442

mean 0.579 0.490 0.510 0.517 0.558 0.571 0.568

recovery 116.0 98.0 102.0 103.4 111.5 114.3 113.6

RE [%] 16.0 7.5 7.6 8.5 21.8 20.0 19.4

CV [%] 15.7 10.0 9.3 10.2 21.7 18.5 17.8

0,0

10,0

20,0

30,0

40,0

50,0

60,0

70,0

80,0

PL (5-

30ng/mL)

PL (0.75-

100ng/mL)

4PL (0.75-

100ng/mL)

5PL (0.75-

100ng/mL)

PL (6.8-

80ng/mL)

4PL (6.8-

80ng/mL)

5PL (6.8-

80ng/mL)

acti

vit

y [

%]

Page 65: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

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65

Results with an expected activity of 100% varied between 98.5% and 106.0% recovery with REs

between 3.4% and 10.9% and CVs between 4.8% and 15.3%. They are shown in table 4 and figure

16.

Table 4. Results CTLL-2 potency assay: expected activity 100% (i.e. relative potency: 1.0).

-

PL

(5-

30ng/

mL)

PL

(0.75-

100ng/

mL)

4PL

(0.75-

100ng/mL)

5PL

(0.75-

100ng/mL)

PL

(6.8-

80ng/mL)

4PL

(6.8-

80ng/mL)

5PL

(6.8-

80ng/mL)

Result assay 1 1.167 1.010 0.98 1.01 1.048 1.028 1.029

Result assay 2 1.065 0.979 failed failed 0.808 0.861 0.86

Result assay 3 1.142 0.941 failed failed 0.997 1.008 1.003

Result assay 4 0.986 1.212 1.07 1.101 0.857 1.022 1.022

Result assay 5 1.030 0.964 0.99 0.975 1.233 1.045 1.046

Result assay 6 0.968 0.93 failed failed 0.968 1.018 1.019

mean 1.059 1.006 1.012 1.028 0.985 0.997 0.997

recovery 106.0 100.6 101.2 102.9 98.5 99.7 99.7

RE [%] 7.5 6.8 3.4 4.5 10.9 4.3 4.3

CV [%] 7.7 10.4 4.8 6.3 15.3 6.8 6.9

Figure 16. Results CTLL-2 potency assay: expected activity 100%. Mean values of six repetitions are shown for each concentration range and analysis model. Error bars indicate the mean CVs. The red, dashed line demonstrates the expected activity of 100%.

0,0

20,0

40,0

60,0

80,0

100,0

120,0

0 PL (5-

30ng/mL)

PL (0.75-

100ng/mL)

4PL (0.75-

100ng/mL)

5PL (0.75-

100ng/mL)

PL (6.8-

80ng/mL)

4PL (6.8-

80ng/mL)

5PL (6.8-

80ng/mL)

acti

vit

y [

%]

Page 66: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

IV. RESULTS AND DISCUSSION

66

0,0

20,0

40,0

60,0

80,0

100,0

120,0

140,0

160,0

180,0

200,0

PL (5-

30ng/mL)

PL (0.75-

100ng/mL)

4PL (0.75-

100ng/mL)

5PL (0.75-

100ng/mL)

PL (6.8-

80ng/mL)

4PL (6.8-

80ng/mL)

5PL (6.8-

80ng/mL)

acti

vit

y [

%]

Results with an expected activity of 150% varied between 96.3% and 106.9% recovery with REs

between 5.3% and 19.5% and CVs between 6.5% and 22.6%. They are shown in table 5 and figure

17.

Table 5. Results CTLL-2 potency assay: expected activity 150% (i.e. relative potency: 1.5).

-

PL

(5-

30ng/mL)

PL

(0.75-

100ng/

mL)

4PL

(0.75-

100ng/

mL)

5PL

(0.75-

100ng/mL)

PL

(6.8-

80ng/mL)

4PL

(6.8-

80ng/mL)

5PL

(6.8-

80ng/mL)

Result assay 1 1.762 1.493 failed 1.495 2.075 1.774 1.777

Result assay 2 1.469 1.13 1.342 1.347 1.205 1.272 1.263

Result assay 3 1.537 1.754 1.633 failed 2.005 failed failed

Result assay 4 1.397 1.553 1.554 1.549 1.335 1.482 1.481

Result assay 5 1.43 1.59 failed failed 1.393 1.477 1.441

Result assay 6 1.351 1.433 1.38 1.388 1.607 failed failed

mean 1.491 1.492 1.477 1.445 1.603 1.501 1.491

recovery 99.4 99.5 98.4 96.3 106.9 100.1 99.4

RE [%] 7.2 9.3 5.8 5.3 19.5 9.1 9.9

CV [%] 9.9 14.0 9.5 6.5 22.6 13.8 14.3

Figure 17. Results CTLL-2 potency assay: expected activity 150%.

Mean values of six repetitions are shown for each concentration range and analysis model. Error bars indicate the mean CVs. The red, dashed line demonstrates the expected activity of 150%.

Page 67: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

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67

In general, results were slightly more accurate and precise at a target concentration of 100% in

comparison to the target concentrations of 50% and 150%. Nevertheless, results were – except

some individual results of 50% and 150% - all lying inside in the acceptable range of ± 30%, which

is the applied QC criterion at Merck Serono for bioassays.

Regarding the accuracies of the mean values (including all results), no major differences between

the three models were observed, even if the mean RE was a bit higher for the PL model than for

the logistic models. However, the logistic models were more precise than the PL model. For the PL

model, a mean coefficient of variance of 14.1% (n = 54 assays) was calculated in contrast to 10.4%

for the 4PL model (n = 36 assays) and 10.3% for the 5PL model (n = 36 assays). This was due to

the fact, that individual results of the logistic models were more accurate than those of the PL

model in particular for results having a large deviation from the expected activity.

According to the statistical analysis performed, the data were normally distributed (KS-test: p =

0.07). Neither for the standard deviations (C-test: p = 0.05) nor for the mean values (ANOVA: p =

0.83) significant differences were observed. This was also applicable when individual data - e.g.

results from one plate analyzed using all three models – were considered (data not shown). For the

three concentration levels 50%, 100% and 150% and for the different concentration ranges A, B

and C, the KW-test was applied, because standard deviations differed significantly (C-test: p <

0.05). Similar to the analysis of the overall results, this test did not show any significant difference

between the different models (KW-test on concentration levels: p = 0.12; KW-test on concentration

ranges: p = 0.23).

The statistical similarity of the results of the different concentration levels 50%, 100% and 150%

underlined that the different models worked appropriately over the whole range between 50% and

150% of the sample concentration in comparison to the standard. Results were not only accurate

and precise at sample concentrations near to the standard concentration, but also at

concentrations which differed more from the expected standard concentration, at the end of the

tested assay range (50% and 150%).

The statistical similarity of the results of the different concentration ranges A, B and C lead to the

assumption that the choice of the concentration range seemed not to be essentially important.

Even if the curve parameters were not derived from the mass action law or other reaction

equations, but from shape fitting only, accurate and precise results were obtained for all of the

models and all concentration ranges selected. Thus, there was no significant difference between

the results of the very close range A having almost all concentration points in the linear range of

the curve and the results of the wide range B having only three points in the concentration

dependent region of the curve.

More eye-catching than the differences in accuracy and precision was in contrast the failure rate of

the different models including all assays with failed tests of linearity or parallelism according to

preset acceptance criteria.

Page 68: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

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68

While all assays were valid for the PL model, failure rates of 27.8% for the 4PL model (ten out of 36

assays, two of these due to lack of linearity and eight of these due to lack of parallelism) and 30.6%

for the 5PL model (eleven out of 36 assays, one of these due to lack of linearity and ten of these

due to lack of parallelism) were noticed, resulting in a significant difference between the PL model

(p < 0.05) and the logistic models based on the failure rate mean of 16.7%.

An overall summary of the CTLL-2 assay results is shown in table 6.

Table 6. Summary of CTLL-2 assay results.

Concentration

range; dilution

factor

Analysis

model

Activity

expected

[%]

Activity

measured

(range)

[%]

Mean

activity

measured

[%]

Recovery

[%]

RE

[%]

CV

[%]

n

(valid

assays out

of six

repetitions)

5-30ng/mL; 1.25 PL

50

50.0 – 73.3 58.0 116.0 16.0 15.7 6

0.75-100ng/mL;

1.85

PL 43.1 – 57.5 49.0 98.0 7.5 10.0 6

4PL 46.0 – 57.0 51.0 102.0 7.6 9.3 5

5PL 46.2 – 57.9 51.7 103.4 8.5 10.2 4

6.8-80ng/mL; 1.36

PL 42.9 – 73.7 55.8 111.5 21.8 21.7 6

4PL 44.3 – 70.0 57.1 114.3 20.0 18.5 4

5PL 44.2 – 68.8 56.8 113.6 19.4 17.8 4

5-30ng/mL; 1.25 PL

100

96.8 – 116.7 106.0 106.0 7.5 7.7 6

0.75-100ng/mL;

1.85

PL 93.0 – 121.2 100.6 100.6 6.8 10.4 6

4PL 98.0 – 107.0 101.2 101.2 3.4 4.8 3

5PL 97.5 – 110.1 102.9 102.9 4.5 6.3 3

6.8-80ng/mL; 1.36

PL 80.8 – 123.3 98.5 98.5 10.9 15.3 6

4PL 86.1 – 104.5 99.7 99.7 4.3 6.8 6

5PL 86.0 – 104.6 99.7 99.7 4.3 6.8 6

5-30ng/mL; 1.25 PL

150

135.1 – 176.2 149.1 99.4 7.2 9.9 6

0.75-100ng/mL;

1.85

PL 113.0 – 175.4 149.2 99.5 9.3 14.0 6

4PL 134.2 – 163.3 147.8 98.4 5.8 9.5 4

5PL 134.7 – 154.9 144.5 96.3 5.3 6.5 4

6.8-80ng/mL; 1.36

PL 120.7 – 207.5 160.3 106.9 19.5 22.6 6

4PL 127.2 – 177.4 150.1 100.1 9.1 13.8 4

5PL 126.3 – 177.7 149.1 99.4 9.9 14.3 4

Page 69: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

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69

1.2. DiFi potency assay

1.2.1. Concentration ranges

The DiFi potency assay measures the inhibitory activity of anti-EGFR antibodies by impeded cell

proliferation of EGFR positive cells.

The assay was performed as described under Materials and Methods. Similar to the CTLL-2 assay,

the DiFi assay was equally performed on three different concentration ranges: a narrow range A (2-

12nM, see figure 18A) with the aim to place as many points as possible in the linear range of the

curve, a wide range B (0.25-95nM, see figure 18B) with the aim to have three points each in the

minimal, linear and maximal range of the curve and an intermediate range C (5-55nM, see figure

18C).

Standard Curve

0

0,1

0,2

0,3

0,4

0,5

0,6

0,7

0,8

1 10 100

x

y

Concentration [nM]

OD

valu

es

at

490

nm

A

Standard Curve

0

0,1

0,2

0,3

0,4

0,5

0,6

0,7

0,8

0,9

0,1 1 10 100 1000

x

y

OD

va

lue

s a

t 4

90

nm

B

Concentration [nM]

Page 70: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

IV. RESULTS AND DISCUSSION

70

Standard Curve

0

0,1

0,2

0,3

0,4

0,5

0,6

0,7

0,8

0,9

1

1 10 100

x

y

Concentration [nM]

OD

va

lue

s a

t 4

90

nm

C

Figure 18. Concentration ranges of the DiFi potency assay. The assay was performed on three different concentration ranges convenient for the different analysis models. The resulting, representative curves are shown: a close range A (2-12nM, see figure 18A), a wide range B (0.25-95nM, see figure 18B) and an intermediate range C (5-55nM, see figure 18C). Green points indicate the individual results, red points the mean values of the triplicates.

1.2.2. Test on the necessity of “weighting”

In order to investigate whether weighting was necessary in case of the DiFi assay, we made the

same calculations according to DeSilva et al. (2003) and the USP (2001) as for the CTLL-2

potency assay. The pertaining illustrations are shown in figures 20 and 21.

According to the calculations proposed by DeSilva et al. (see figure 19), again, a slight trend to

increasing SDs at increasing responses could be noted in some of our curves, which was however

again not consistent through the whole range (since SDS increased first and than remained

constant or even decreased again).

A

DiFi assay: concentration range 2 - 12nM

y = -0,1037x - 1,3702

R2 = 0,0357

-2,5

-2

-1,5

-1

-0,5

0

0 0,2 0,4 0,6 0,8 1

absorbance

log

[sta

nd

ard

devia

tio

n]

Page 71: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

IV. RESULTS AND DISCUSSION

71

B

DiFi assay: concentration range 0,25 - 95.5nM

y = 0,7858x - 2,0106

R2 = 0,5711

-2,5

-2

-1,5

-1

-0,5

0

0 0,2 0,4 0,6 0,8 1

absorbance

log

[sta

nd

ard

devia

tio

n]

C

DiFi assay: 5 - 55nM

y = 0,9397x - 2,0963

R2 = 0,6215

-2,5

-2

-1,5

-1

-0,5

0

0 0,2 0,4 0,6 0,8 1

absorbance

log

[sta

nd

ard

devia

tio

n]

Figure 19. Plot of the pooled standard deviations (n = 18) vs. the measured mean responses for each concentration point. Illustrations are given for the different concentration ranges of the DiFi potency assay (fig. 19A: 2-12nM; fig. 19B: 5-55nM; fig. 19C: 0.25-95nM). According to DeSilva (2003), weighting is appropriate, if a plot of the pooled standard deviations vs. the mean responses reveals a linearly increasing relationship on a logarithmic scale.

According to the calculations proposed by the USP (see figure 20), the data followed approximately

a straight line, which was in all three cases even slightly decreasing.

Page 72: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

IV. RESULTS AND DISCUSSION

72

A

DiFi assay: concentration range 2 - 12nM

y = -0,0002x - 1,4107

R2 = 0,0153

-2,5

-2

-1,5

-1

-0,5

0

0 20 40 60 80 100 120 140

dose squared

log

[sta

nd

ard

devia

tio

n]

B

DiFi assay: concentration range 0,25 - 95.5nM

y = -7E-05x - 1,6244

R2 = 0,4267

-2,5

-2

-1,5

-1

-0,5

0

0 2000 4000 6000 8000 10000

dose squared

log

[sta

nd

ard

devia

tio

n]

C

DiFi assay: 5 - 55nM

y = -0,0002x - 1,5457

R2 = 0,6223

-2,5

-2

-1,5

-1

-0,5

0

0 500 1000 1500 2000 2500 3000 3500

dose squared

log

[sta

nd

ard

devia

tio

n]

Figure 20. Plot of the pooled standard deviations (n = 18) vs. the dose squared for each concentration point. Illustrations are given for the different concentration ranges of the DiFi potency assay (fig. 20A: 2-12nM; fig. 20B: 5-55nM; fig. 20C: 0.25-95nM). According to the USP, weighting is recommended, when the plot of the sample variance is proportionally increasing to a function of dose, e.g. dose squared. If the data follow a horizontal line, no weighting is needed.

Page 73: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

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73

As a consequence, unweighted regressions were used in this study for all concentration ranges of

the DiFi potency assay.

1.2.3. Results

Results of the DiFi assay for the PL model, 4PL model and 5PL model varied between 75.6% and

147.6% recovery, those of the 4PL model between 81.8% and 125.4% recovery and those of the

5PL model between 79.9% and 125.4% recovery, respectively. A mean accuracy of 97.2%

(recovery) 11.8% (mean RE) was obtained using the PL model, whereas accuracies of 99.4%

7.1% and 99.1% 7.3% were assessed for the 4PL and 5PL model, respectively. As an example,

individual, representative graphs are shown in figure 21.

Figure 21. Individual, representative graphs (calculated by PLA) of a DiFi potency assay. Results of an assay with a target concentration of 100%, analyzed by the PL model (see figure 21A), the 4PL model (see figure 21B) and the 5PL model (see figure 21C) are shown.

Results with an expected activity of 50% varied between 95.3% and 99.9% recovery with REs

between 7.8% and 18.8% and CVs between 12.3% and 25.6%. The recoveries obtained are

summarized in table 7 and figure 22.

A B CA B C

Page 74: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

IV. RESULTS AND DISCUSSION

74

Table 7. Results DiFi potency assay: expected activity 50% (i.e. relative potency: 0.5).

Figure 22. Results DiFi potency assay: expected activity 50%. Mean values of six repetitions are shown for each concentration range and analysis model. Error bars indicate the mean CVs. The red, dashed line demonstrates the expected activity of 50%.

Results with an expected activity of 100% varied between 92.4% and 99.2% recovery with REs

between 3.8% and 12.4% and CVs between 5.3% and 13.4%. They are shown in table 8 and figure

23.

-

PL

(2-

12nM)

PL

(0.25-

95nM)

4PL

(0.25-

95nM)

5PL

(0.25-

95nM)

PL (5-

55nM)

4PL (5-

55nM)

5PL (5-

55nM)

Result assay 1 0.430 0.467 0.461 0.464 0.615 0.609 0.608

Result assay 2 0.738 0.413 0.409 0.396 0.472 0.484 0.482

Result assay 3 0.436 0.522 0.52 0.522 0.380 0.466 0.464

Result assay 4 0.420 0.626 0.627 0.627 0.528 0.509 0.505

Result assay 5 0.442 0.488 failed failed 0.378 0.426 0.437

Result assay 6 0.447 0.411 0.44 0.44 0.487 0.502 0.497

mean 0.486 0.488 0.491 0.490 0.477 0.500 0.499

recovery 97.1 97.6 98.3 98.0 95.3 99.9 99.8

RE [%] 18.8 12.3 13.5 14.0 14.2 8.1 7.8

CV [%] 25.6 16.5 17.5 18.2 18.9 12.3 20.2

0,0

10,0

20,0

30,0

40,0

50,0

60,0

70,0

80,0

PL (2-12nM) PL (0.25-

95nM)

4PL (0.25-

95nM)

5PL (0.25-

95nM)

PL (5-55nM) 4PL (5-

55nM)

5PL (5-

55nM)

ac

tiv

ity

[%

]

Page 75: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

IV. RESULTS AND DISCUSSION

75

Table 8. Results DiFi potency assay: expected activity 100% (i.e. relative potency: 1.0).

- PL (2-

12nM)

PL

(0.25-

95nM)

4PL

(0.25-

95nM)

5PL

(0.25-

95nM)

PL (5-

55nM)

4PL (5-

55nM)

5PL (5-

55nM)

Result assay 1 0.963 0.936 0.972 0.946 1.033 1.04 1.042

Result assay 2 1.064 1.159 1.041 1.03 1.035 1.03 1.038

Result assay 3 0.941 0.942 failed failed 0.875 0.888 0.886

Result assay 4 0.925 0.839 0.943 0.909 1.000 failed failed

Result assay 5 0.877 0.897 0.904 0.9 0.988 1.003 1.000

Result assay 6 0.773 0.804 0.946 0.94 0.973 0.993 0.993

mean 0.924 0.930 0.962 0.945 0.984 0.991 0.992

recovery 92.4 93.0 96.1 94.5 98.4 99.1 99.2

RE [%] 9.8 12.4 5.5 6.7 3.9 3.8 4.0

CV [%] 10.4 13.4 5.3 5.4 9.3 6.1 6.4

Figure 23. Results DiFi potency assay: expected activity 100%.

Mean values of six repetitions are shown for each concentration range and analysis model. Error bars indicate the mean CVs. The red, dashed line demonstrates the expected activity of 100%.

Results with an expected activity of 150% varied between 92.4% and 99.2% recovery with REs

between 4.3% and 14.7% and CVs between 5.8% and 18.5%. They are shown in table 9 and figure

24.

0,0

20,0

40,0

60,0

80,0

100,0

120,0

PL (2-

12nM)

PL (0.25-

95nM)

4PL (0.25-

95nM)

5PL (0.25-

95nM)

PL (5-

55nM)

4PL (5-

55nM)

5PL (5-

55nM)

acti

vit

y [

%]

Page 76: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

IV. RESULTS AND DISCUSSION

76

Table 9. Results DiFi potency assay: expected activity 150% (i.e. relative potency: 1.5).

- PL (2-

12nM)

PL

(0.25-

95nM)

4PL

(0.25-

95nM)

5PL

(0.25-

95nM)

PL (5-

55nM)

4PL (5-

55nM)

5PL (5-

55nM)

Result assay 1 1.468 1.32 1.557 failed 1.418 1.443 1.435

Result assay 2 1.424 1.834 1.681 1.727 1.484 1.438 1.442

Result assay 3 1.581 1.356 failed failed 1.291 1.365 1.402

Result assay 4 1.211 1.625 1.56 1.56 1.270 failed failed

Result assay 5 1.448 1.924 1.48 1.494 2.016 1.728 1.704

Result assay 6 1.66 1.382 1.502 1.515 1.420 1.461 1.483

mean 1.465 1.573 1.556 1.574 1.483 1.487 1.493

recovery 97.7 104.9 103.7 104.9 98.9 99.1 99.5

RE [%] 7.7 14.7 4.3 5.1 12.6 6.9 5.9

CV [%] 10.5 16.6 5.8 6.7 18.5 9.4 8.1

Figure 24. Results DiFi potency assay: expected activity 150%. Mean values of six repetitions are shown for each concentration range and analysis model. Error bars indicate the mean CVs. The red, dashed line demonstrates the expected activity of 150%.

For the DiFi assay, in general, the same tendencies as for the CTLL-2 potency assay were

observed. The mean RE and thus the accuracy of the assay was slightly better for the logistic

models, but not significantly different. The precision of the PL model was with a coefficient of

variation of 15.1% (n = 54 assays) again lower as those of the 4PL and 5PL model with 9.4% (n =

36 assays). As before no significant difference could be noted between the mean values: according

0,0

20,0

40,0

60,0

80,0

100,0

120,0

140,0

160,0

180,0

200,0

PL (2-

12nM)

PL (0.25-

95nM)

4PL

(0.25-

95nM)

5PL

(0.25-

95nM)

PL (5-

55nM)

4PL (5-

55nM)

5PL (5-

55nM)

acti

vit

y [

%]

Page 77: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

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77

to the performed ANOVA test, a p-value of 0.68 was calculated. Since data were not normally

distributed in this case (KS-test: p = 0.02), the Levene‟s test was performed for variance check of

the standard deviations (L-test: p = 0.13).

Also neither for the individual values (data not shown), nor for the different concentration levels

(KS-test: p = 0.17, C-test: p < 0.05, KW-test: p = 0.14), nor for the different concentration ranges

(KS-test: p = 0.009, L-test: p = 0.41, ANOVA test: p = 0.63) a significant difference was observed.

As a consequence, for both assays neither the selected concentration level (50%, 100% or 150%),

nor the chosen concentration range (e.g. closer or wider range) had a statistically significant impact

on the result of the assay.

For the DiFi assay, a higher failure rate of the 4PL and 5PL model in comparison to the PL model

was observed. This finding was comparable to the results of the CTLL-2 assay. All performed

assays for the PL model were valid, whereas the logistic assays showed a higher failure rate

(definition see section II.2.4.3.), which was again significantly different from that of the PL model.

The failure rate of the 5PL model was with 16.7% (six out of 36 assays, three of these due to lack

of parallelism and three of these due to lack of linearity and parallelism) again slightly more

elevated as for the 4PL model with 13.9% (five out of 36 assays, two of these due to lack of

linearity, one of these due to lack of parallelism and two of these due to lack of both). This

difference between the logistic models was however not statistically significant.

An overall summary of the DiFi assay results is shown in table 10.

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Table 10. Summary of DiFi assay results.

Concentration

range; dilution

factor

Analysis

model

Activity

expected

[%]

Activity

measured

(range)

[%]

Mean

activity

measured

[%]

Recovery

[%]

RE

[%]

CV

[%]

n

(valid

assays out

of six

repetitions)

2-12nM; 1.25 PL

50

42.0 – 73.8 48.6 97.1 18.8 25.6 6

0.25-95nM; 2.1

PL 41.1 – 63.2 48.8 97.6 12.3 16.5 6

4PL 40.9 – 62.7 49.1 98.3 13.5 17.5 5

5PL 39.6 – 62.7 49.0 98.0 14.0 18.2 5

5-55nM; 1.35

PL 37.8 – 61.5 47.7 95.3 14.2 18.9 6

4PL 42.6 – 60.9 49.9 99.9 8.1 12.3 6

5PL 43.7 – 60.8 49.9 99.8 7.8 11.8 6

2-12nM; 1.25 PL

100

77.3 – 106.4 92.4 92.4 9.8 10.4 6

0.25-95nM; 2.1

PL 80.4 – 115.9 93.0 93.0 12.4 13.5 6

4PL 90.4 – 104.1 96.1 96.1 5.5 5.3 5

5PL 90.0 – 103.0 94.5 94.5 6.7 5.4 5

5-55nM; 1.35

PL 87.5 – 103.5 98.4 98.4 3.9 9.3 6

4PL 88.8 – 104.0 99.1 99.1 3.8 6.1 5

5PL 88.6 – 104.2 99.2 99.2 4.0 6.4 5

2-12nM; 1.25 PL

150

121.1 – 166.0 146.5 97.7 7.7 10.5 6

0.25-95nM; 2.1

PL 132.0 – 192.4 157.4 104.9 14.7 16.6 6

4PL 148.0 – 168.1 155.6 103.7 4.3 5.0 5

5PL 149.1 – 172.7 157.4 104.9 5.1 6.7 4

5-55nM; 1.35

PL 127.0 – 201.6 148.3 98.9 12.6 18.5 6

4PL 136.5 – 172.8 148.7 99.1 6.9 9.4 5

5PL 140.2 – 170.4 149.3 99.5 5.9 8.1 5

1.3. Combined discussion of CTLL-2 and DiFi potency assays results

Already in the 1970s, the question of the right analysis model for bioassays was discussed. Thus

different mathematical methods for calculation of radioimmunoassay results were compared

(Sandel and Vogt, 1978; Rodbard et al., 1978). Rodgers (1984) summarized most of the methods

known to this time and also raised the question for the best model. To date no clear

recommendation for the right choice of analysis model can be given, since it depends on the

experimental setup and each of the methods possesses its advantages and disadvantages.

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However, it was already shown that results varied by using different calculation models (Jeffcoate

and Das, 1977; Pegg and Miner, 1982).

In this study, no significant difference was observed between the PL, 4PL and 5PL models

regarding accuracy and precision. Nevertheless, small differences between the models could be

noticed. For both assay types, the precision of the logistic models was with a CV of approximately

10% higher than that of the PL model with a CV of approximately 15%. This was the same for the

accuracy with a mean RE of 7 - 8% for the logistic models versus 12% for the PL model. Similar

results have already been observed by Plikaytis (1991), who compared different models (log-log

model, two forms of the logit-log model and 4PL) for quantification of Neisseria meningitides Group

A Polysaccharide Antibody Levels by ELISA. They noted even larger differences between the

different models as in our case. The calculated precisions were 21.6% (n = 7) for the log-log model,

which was the least precise of the four methods compared, in contrast to 3.0% (n = 7) for the 4PL

model, being the most precise of the four methods.

A reason for the higher accuracy and precision of the logistic models might be the better assurance

of similarity between sample and reference, because the entire curve is considered for potency

calculation and not only the linear part as for the PL model (Findlay and Dillard, 2007).

Consequently, more data points are used. Moreover, during linearization of the curve, an

underlying bias might be inserted which could lead to the lacking precision of the PL model (Findlay

and Dillard, 2007; Rodgers, 1984). This bias is dependent upon concentration: It is greatest at the

ends of the assay range, which explains the larger deviations from the target concentrations at

concentration levels of 50% and 150%, in comparison to the concentration level of 100%.

For both assay types, the failure rate of the logistic models was more elevated and significantly

different from that of the PL model. Thereby, the failure rate of the 5PL model was even higher then

that of the 4PL model. This observation is supported by Findlay and Dillard (2007), who advice to

use the 5PL model only in cases with a clear asymmetry of the curve since in other cases the

additional fifth parameter might destabilize the fitting algorithm.

This would lead to the conclusion that the 4PL model fitted the curve better than the 5PL model,

e.g. the differences between the observed data and the fitted regression were smaller for the 4PL

model.

In order to further explore which model fitted the CTLL-2 and DiFi data better, the mean RE [(back

calculated – nominal concentration)/nominal concentration*100] was calculated for each individual

concentration, which gives a measure of the goodness of fit for each model (Findlay and Dillard,

2007). For backcalculation of the concentration points, the equations of the 4PL and 5PL model

were used, described in the Introduction section I.3.3.2.2.

The pertaining illustrations of the mean REs over the different concentration points are shown in

figure 25.

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A

CTLL-2 assay: concentration range 0.75 - 100ng/mL

-25

-20

-15

-10

-5

0

5

10

15

20

25

10054,0529,215,88,554,62,51,350,75

dose

%R

E [

resid

uals

/measu

red

resp

on

se*1

00]

4PL

5PL

B

CTLL-2 assay: concentration range 6.8 - 80ng/mL

-25

-20

-15

-10

-5

0

5

10

15

20

25

8058,843,315,823,417,212,59,36,8

dose

%R

E [

resid

uals

/measu

red

resp

on

se*1

00]

4PL

5PL

C

DiFi assay: concentration range 0.25 - 95.5nM

-25

-20

-15

-10

-5

0

5

10

15

20

25

0,25 54,05 1,1 15,8 4,9 10,2 21,4 45 95,5

dose

%R

E [

resid

uals

/measu

red

resp

on

se*1

00]

4PL

5PL

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D

DiFi assay: concentration range 5 - 55nM

-25

-20

-15

-10

-5

0

5

10

15

20

25

5 54,05 9,1 15,8 16,6 22,4 30,3 40,9 55,2

dose

%R

E [

resid

uals

/measu

red

resp

on

se*1

00]

4PL

5PL

Figure 25. % REs [residuals/ measured response*100] of the 4PL and 5PL models for each concentration point. Residuals are the difference between the backcalculated and nominal concentration. The smaller the residuals and the % REs are, the better is the curve fit of the model. Illustrations are given for the different concentration ranges of the CTLL-2 (fig. 27A: 0.75–100ng/mL; fig. 27B: 6.8-80ng/mL) and DiFi (fig. 27C: 5-55nM; fig. 27D: 0.25-95nM) potency assays.

Visual inspection of figure 25 and calculation of the mean RE over all concentration points showed

that the two models were approximately equivalent for the concentration range 0.75–100ng/mL of

the CTLL-2 potency assay (see figure 25A) and the concentration range 5–55nM of the DiFi

potency assay (see figure 25D). The mean REs for the 4PL and 5PL models were 6.5% and 6.4%

(CTLL-2 assay) as well as 9.8% and 10.5% (DiFi assay), respectively. For the concentration range

0.25–95nM of the DiFi potency assay, the 4PL model fitted the curve better with a mean RE of

8.9% in comparison to 14.3% of the 5PL model (see figure 25C). In contrast, in case of the

concentration range 6.8-80ng/mL of the CTLL-2 potency assay, the fit of the 5PL model was with

7.3% RE better than those of the 4PL model with 14.4% RE (see figure 25B). This was in good

agreement with the shapes of the curves since by visual inspection of the curves, this latter curve

seemed to be asymmetric since the lower plateau of the curve was missing (see figure 13C). In

opposition to this, the other three curves (see figures 13 and 20) seemed to be symmetric.

Interestingly, the results of the calculated potencies were not influenced by the fits of the models.

Even if one of the models fitted the curve better, hardly any differences were noticed in the

calculated potencies.

The higher failure rate of the logistic models in comparison to the PL model supports the discussion

about the appropriate test of similarity, which is currently on-going between the USP and the Ph.

Eur. The Ph. Eur. recommends using the difference test (F-test) - an ANOVA test - whereas the

USP advices to use an equivalence test. The problem of the ANOVA technique, which was also

used in this case, is that it is hyper-sensitive, even to negligible deviations from parallelism. This is

especially the case for models with a very high precision. In those cases, a slight difference

between the sample and the reference standard will already be denoted as statistically different by

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the ANOVA technique. The ability to detect lack of satisfactory “goodness-of-fit” for a curve

improves since the precision of the assay improves (Dudley et al., 1985). As a consequence, the

more precise the assay is, the higher the possibility is to fail the test of parallelism. This could

explain the higher failure rate of the logistic models in comparison to the PL model, observed

during this study. Likewise, the higher the number of replicates and the higher the number of dose

levels is, the higher the possibility is to detect lack of fit, and hence may introduce the need to

utilize more complex models. Conversely, when experimental errors are large, and replicates are

few, simple models are likely to be “adequate” (Dudley et al., 1985).

In order to solve the problem of the high failure rate of the logistic models, an alternative

equivalence test was proposed to the ANOVA test (Story et al., 1986). This test determines a

critical value for parallelism mean by multiplying the appropriate critical F value for parallelism by

the value for error mean square, providing a limiting value for the fiducial limits. This approach

should enable to improve bioassay technique by accepting precise assays but not doubtful assay

results. The equivalence test is discussed as alternative to the ANOVA test, but is also not free of

criticisms (Draper and Smith, 1998; Bates and Watts, 1988).

The problem of the right test of parallelism has also already been discussed by Plikaytis et al.

(1994), who developed seven guidelines applicable to most immunoassays, which should serve as

an alternative to the standard ANOVA technique. Other proposals are the weighted-sum-of-

squares regression (Gottschalk and Dunn, 2005, a) and the testing of the null hypothesis for a

specified difference between the slopes of two bioassay curves (Callahan and Saijadi, 2003;

Plikaytis and Carlone, 2005).

It still needs to be determined which of the tests mentioned above is the most advantageous. In

any case, by replacing the ANOVA test by one of them, the failure rate of the logistic models might

be reduced.

Another factor which might influence the decision for a specific analysis model is the number of

dilution steps on a plate. In this study, nine dilution steps were used for all three models, PL, 4PL

and 5PL; there was consequently no difference in the workload of the different assays. However,

whilst all of the nine steps are definitely required for the logistic models, a reduction of the dilution

steps is possible for the PL model since it usually only uses three to four steps in the linear range

of the curve. In an additional study, the number of dilutuion steps was reduced to three and four

steps, respectively. Reduction to three dilution steps was not possible due to a too high number of

failed assays; however satisfactory results were obtained by using four dilutions steps (data not

shown). As a conclusion of this reduction from nine to four dilution steps, three samples could be

analyzed on one plate only, reducing the workload considerably. This fact favours the use of the PL

model.

1.4. Summary and Conclusions

This study is a systematic and thorough comparison addressing the question of potency assay

evaluation by different analysis models using actual data of two different bioassays.

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In summary, this study showed that no significant differences regarding accuracy and precision

between the three different models for potency assay calculation were observed, neither for the

CTLL-2 assay (ANOVA test: p = 0.83), nor for the DiFi assay (ANOVA test: p = 0.68).

All important parameters of both assays are summarized in table 11.

Table 11. Summary and comparison between the different models.

Criteria Assay type PL 4PL 5PL

Total amount of

analyzed assays

CTLL-2 54 36 36

DiFi 54 36 36

Accuracy

(Recovery ± RE)

[%]

CTLL-2 104.0 11.8 102.4 8.5 102.3 8.5

DiFi 97.2 11.8 99.4 7.1 99.1 7.3

Precision [%] CTLL-2 14.1 10.4 10.3

DiFi 15.1 9.4 9.4

Failure rate [%]

(n)

CTLL-2 0

(0)

27.8

(10)

30.6

(11)

DiFi 0

(0)

13.9

(5)

16.7

(6)

The logistic models show a slightly better accuracy and precision in comparison to the PL model, in

exchange, they have a higher failure rate, which differs significantly from that of the PL model.

These parameters have to be balanced during the model selection process in method

development. Moreover, it has to be considered on the one hand, that the PL model is more

precisely described in the Ph. Eur., chapter 5.3 and that applying this model can reduce the

number of concentration levels and workload. On the other hand, the better assurance of similarity

between sample and reference, leading to a higher accuracy and precision of the logistic models

needs to be accounted for. Also the possibility of the application of an alternative similarity test

(instead of the F-test) should be taken into consideration, because this might reduce the failure rate

of the logistic models.

Above this, it has always to be kept in mind that the appropriate model depends on the performed

type of assay set up.

Thus, the preferred model has to be chosen individually. Since there were no significant differences

regarding accuracy and precision and since the failure rate of the logistic models was much higher

than for the PL model, I decided to use further on the PL model for the following studies described

in this thesis.

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2. COMPARISON OF DIFFERENT PROLIFERATION ASSAYS (COLORIMETRIC, LUMINESCENCE AND

FLUORESCENCE READ-OUTS)

Some of the most commonly used read-out systems for potency assays to date are based on

colorimetric, luminescence or fluorescence reactions. At the Bioassay laboratory at Merck Serono,

the colorimetric system, utilizing the tetrazolium salt and MTT analogue MTS/PMS, was originally

used for detection of all kinds of proliferation assays. MTS is a tetrazolium salt, which is reduced to

an intensely colored formazan by the mitochondria enzymes of living cells (Goodwin et al., 1995).

PMS acts as an intermediate electron acceptor and accelerates the reaction. The amount of the

produced formazan is direct proportional to the number of living cells in culture and can be

measured at 492nm (Malich et al., 1997).

In this study, it was investigated, whether alternative luminescence or fluorescence reagents were

more advantageous in comparison to the colorimetric system and which system was the most

favourable for QC purposes.

As an example for a luminescence read-out, CellTiter- Glo® (Promega) was used. This

bioluminescent assay uses an enzyme, luciferase, which catalyzes the formation of light in the

presence of ATP and luciferin. The emitted light intensity correlates with the amount of ATP

present and consequently provides a direct measure of the number of viable cells (Crouch et al,

1993).

The substrate used for fluorescence measurements was Alamar BlueTM

(Invitrogen). The native,

oxidized form of the Alamar Blue reagent is taken up readily by the cells and is reduced

intracellularly by oxidoreductases and the mitochondrial electron transport chain, with a

corresponding shift in its absorbance and fluorescence (Ahmed et al., 1994; Goegan et al., 1995).

Consequently, the initial dark blue color of the oxidized state changes to a highly fluorescent red

dye, and becomes a direct estimate of the intracellular rate of reduction, and thus a direct estimate

of the viable cell number.

The three reagents were compared to each other regarding their suitability for QC of

biopharmaceuticals. Each of the three read-outs was tested with each of the three cell lines CTLL-

2, DiFi and Kit 225, allowing a thorough and systematic analysis of the advantages and

disadvantages of the proliferation assays.

2.1. Method development

The change from the coloriometric read-out to luminescence or fluorescence detection made, as a

first step, modification of several parameters in comparison to the originally used colorimetric assay

necessary.

Thus, the following parameters were investigated and modified, starting from the original

colorimetric assay (described under Materials and Methods):

Concentration ranges

Incubation times (with substrate)

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Volume of APIs and cells

Cell densities

Modifications were considered successful if the signal to noise ration could be increased (see

figure 26).

Curve

<Plate Layout Settings>

Lu

m

0,01 0,1 1 10 100

0

200000

400000

600000

800000

1000000

1200000

1400000

1600000

1800000

Concentration [ng/mL]

Re

lati

ve li

ghtu

nit

s(R

LU)

Figure 26. Illustration of the signal to noise ratio of a representative dose response curve. As an example, a concentration curve of a CTLL-2 potency assay, detected by luminescence, is shown. The signal to noise ratio is indicated as the ratio of the highest concentration to the control, both marked in red. Blue points indicate the individual results, orange points the mean values of the triplicates.

The resulting adapted parameters are described in the results section for each individual assay

(CTLL-2, DiFi and Kit 225).

Furthermore, it was investigated, whether it was possible to reduce the incubation time without

substrate, since incubation times were very long, especially for the DiFi and the Kit 225 assay,

having both an incubation time of 96h. However, this was not possible neither for luminescence,

nor for fluorescence read-outs, since signal to noise ratios were not stable and not high enough

after shorter incubation times.

Other parameters to be varied during the method development were the right amounts of substrate

for each read-out system and each individual assay and the right sensitivity of the luminescence

reader (not described individually).

2.2. Results

2.2.2. CTLL-2 potency assay

For the CTLL-2 assay, the concentration range of the colorimetric assay was adapted from 6.8 –

80ng/mL to 0.15 – 50ng/mL for the luminescence technique and 0.25 – 100ng/mL for the

fluorescence technique. This was necessary since the originally used concentration range did not

fit well to the luminescence and fluorescence detection. Performing the assay according to the

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86

concentration range used for colorimetric detection (6.8 – 80ng/mL) according to the valid standard

operation procedure (SOP) the following curve was obtained, using the MTS/PMS reagent (see

figure 27):

0

0,2

0,4

0,6

0,8

1

1,2

1 10 100

y

x

Standard Curve

Concentration [ng/mL]

OD

val

ue

sat

49

0nm

Figure 27. Concentration curve of a CTLL-2 potency assay, detected by colorimetric read-out.

An exemplary, resulting concentration curve is shown by using a concentration range of 6.8 – 80ng/mL. Green points indicate the individual results, red points the mean values of the triplicates.

This curve was not appropriate for QC purposes since the lower asymptote was not covered. Thus,

the original colorimetric potency assay was optimized to a concentration range of 1.5 – 50ng/mL

(see figure 28).

0

0,2

0,4

0,6

0,8

1

1,2

1,4

1 10 100

y

x

Standard Curve

Concentration [ng/mL]

OD

val

ue

sat

49

0nm

Figure 28. Optimized curve of a CTLL-2 potency assay, detected by colorimetric read-out.

An exemplary, resulting concentration curve is shown by optimizing the assay to a concentration range of 1.5 – 50ng/mL. Green points indicate the individual results, red points the mean values of the triplicates.

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By using the original concentration range of 6.8 – 80ng/mL, similar curves to the one shown in

Figure 29 were obtained for luminescence and fluorescence techniques:

Curve

<Plate Layout Settings>

Lu

m

1 10 100

2800000

3000000

3200000

3400000

3600000

3800000

4000000

4200000

4400000

4600000

4800000

5000000

Concentration [ng/mL]

Re

lati

ve li

ghtu

nit

s(R

LU)

Figure 29. Concentration curve of a CTLL-2 potency assay, detected by luminescence read-out. An exemplary, resulting concentration curve is shown by using a concentration range of 6.8 – 80ng/mL. Blue points indicate the individual results, orange points the mean values of the triplicates.

Since this concentration range did not fit well, it had to be adapted to 0.15 – 50ng/mL for the

luminescence technique and 0.25 – 100ng/mL for the fluorescence technique (see figures 30 and

31).

Curve

<Plate Layout Settings>

Lu

m

0,01 0,1 1 10 100

0

200000

400000

600000

800000

1000000

1200000

1400000

1600000

1800000

Concentration [ng/mL]

Re

lati

ve li

ghtu

nit

s(R

LU)

Figure 30. Optimized curve of a CTLL-2 potency assay, detected by luminescence read-out. An exemplary, resulting concentration curve is shown by using a concentration range of 0.15 – 50ng/mL. Blue points indicate the individual results, orange points the mean values of the triplicates.

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Curve

<Plate Layout Settings>

53

0/2

5,6

00

/40

0,01 0,1 1 10 100 1000

0

100000

200000

300000

400000

500000

600000

700000

Concentration [ng/mL]

Re

lati

ve fl

uor

esce

nce

un

its

(RFU

)

Figure 31. Optimized curve of a CTLL-2 potency assay, detected by fluorescence read-out. An exemplary, resulting concentration curve is shown by using a concentration range of 0.25 – 100ng/mL. Blue points indicate the individual results, orange points the mean values of the triplicates.

Thus, the luminescence read-out detected approx. ten times lower immunocytokine concentrations

than the colorimetric read-out.

Another parameter to be modified was the used cell amount, e.g. the cell volume and the cell

density. Using luminescence and fluorescence detection, the cell density could be reduced from

5*105 cells/mL to 2.5*10

5 cells/mL and the used cell number, as well as the amount of API, be

reduced from 100µL/well to 50µL/well leading to a four times lower consumption of cells for the

Alamar Blue and ATP assays in contrast to the MTS assay. This reduction was not possible for the

colorimetric read-out since it lead to significant decreases of the OD differences and consequently

to a decrease of the signal to noise ratios.

It can be concluded that both, the Alamar Blue and the ATP bioluminescence assay showed a

considerably higher sensitivity in comparison to the MTS assay. This is in line with previous results

published by Hamid et al. (2004), Petty et al. (1995), Slater (2001) and Weyermann et al. (2005).

Regarding the incubation time with substrate, the luminescence read-out was the fastest of the

three read-outs since the plate could already be measured 5 - 10min after substrate addition. In

contrast, the incubation time with substrate was 2.5 – 3h for the colorimetric system and 24 4h for

fluorescence. The longer incubation time is the most obvious disadvantage of the Alamar Blue

assay in comparison to the ATP assay since it takes a whole day to complete the assay.

An important criterion for the robustness of an assay is the signal to noise ratio. The higher this

ratio, the more robust and precise is the assay because of the steeper slope of the curve. For the

CTLL-2 potency assay, mean ratios of 2.4 for the colorimetric read-out, 7.3 for the fluorescence

read-out and 13.7 for the luminescence read-out were measured, respectively. The highest signal

to noise ratio is thus another advantage of the ATP assay.

The only detriment of the ATP assay is the higher costs for the CellTiter- Glo® reagent.

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In order to evaluate accuracy and precision of the read-outs, three repetitions were performed for

all three read-out systems on three different sample concentrations of 50%, 100% and 150% in

comparison to the 100% standard (n = 9). The repetitions were performed independently on

different days; assays for the different read-out techniques were performed on the same day.

Results are summarized in tables 12 to 14.

Table 12. Results qualification CTLL-2 assay: expected activity 50% (i.e. relative potency: 0.5).

Read-out Colorimetric Luminescence Fluorescence

Result day 1 0.607 0.548 0.588

Result day 2 0.404 0.503 0.602

Result day 3 0.597 0.568 0.425

Mean 0.536 0.540 0.538

Recovery [%] 107.2 107.9 107.7

RE [%] 20.0 7.9 17.7

CV [%] 21.4 6.2 18.3

Table 13. Results qualification CTLL-2 assay: expected activity 100% (i.e. relative potency: 1.0).

Read-out Colorimetric Luminescence Fluorescence

Result day 1 1.141 0.985 1.043

Result day 2 0.956 1.053 0.966

Result day 3 1.115 1.050 1.059

Mean 1.071 1.029 1.023

Recovery [%] 107.1 102.9 102.3

RE [%] 10.4 3.9 4.5

CV [%] 9.4 3.7 4.9

Table 14. Results qualification CTLL-2 assay: expected activity 150% (i.e. relative potency: 1.5).

Read-out Colorimetric Luminescence Fluorescence

Result day 1 1.783 1.488 1.406

Result day 2 1.411 1.377 1.490

Result day 3 1.499 1.408 1.520

Mean 1.564 1.424 1.472

Recovery [%] 104.3 95.0 98.1

RE [%] 8.3 5.0 2.8

CV [%] 12.4 4.0 4.0

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All results were within the acceptable range of ± 30%, which is usually applied for bioassays at

Merck Seono. Consequently, all read-out systems were qualified.

Regarding the summarized results comprising all three concentration levels of 50%, 100% and

150%, recoveries varied between 80.8% and 119.4% for the colorimetric read-out, 91.8% and

113.6% for luminescence and 85.0% and 120.4% for fluorescence. Mean REs (mean deviations

from the expected activity) of 12.9%, 5.6% and 8.3% were calculated for the colorimetric,

luminescence and fluorescence system, respectively. No major differences between the different

read-out systems regarding accuracy were observed.

The mean CV (13.6%) was slightly higher for the MTS assay in comparison to the Alamar Blue

assay (6.9%) and the ATP assay (4.3%). This observation is consistent with the higher signal to

noise ratios of the latter assays, leading to a higher precision of the assay.

An overall summary of the most important parameters of the CTLL-2 potency assay and a

comparison between the different read-outs is shown in table 15.

Table 15. Summary of CTLL-2 assay parameters and comparison between the different read-out systems.

Read-out Colorimetric Luminescence Fluorescence

Concentration range 1.5 – 50ng/mL 0.15 – 50ng/mL 0.25 – 100ng/mL

Signal to noise ratio, mean

(range)

2.4

(1.8 - 3.2)

13.7

(6 - 22)

7.3

(5 - 9)

Volume of API and cells 100µL/well 50µL/well 50µL/well

Cell density 5*105 cells/mL 2.5*10

5 cells/mL 2.5*10

5 cells/mL

Incubation time (with

substrate)

2.5 – 3h 5 - 10min 24 ± 4h

Recovery (range) 80.8% - 119.4% 91.8% - 113.6% 85.0% - 120.4%

Accuracy

(mean RE [%]; n = 9) 12.9% 5.6% 8.3%

Precision

(Mean CV [%]; n = 9)

13.6% 4.3% 6.9%

Costs/plate (substrate

only)

Luminescence > Fluorescence > Colorimetric

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2.2.3. DiFi potency assay

The DiFi assay was originally performed on a concentration range of 5-55nM (see figure 32).

0

0,1

0,2

0,3

0,4

0,5

0,6

0,7

0,8

0,9

1

1 10 100

y

x

Standard Curve

Concentration [nM]

OD

val

ue

sat

49

0nm

Figure 32. Concentration curve of a DiFi potency assay, detected by colorimetric read-out. An exemplary, resulting concentration curve is shown by using a concentration range of 5- 55nM. Green points indicate the individual results, red points the mean values of the triplicates.

Again, this concentration range was not adequate for luminescence and fluorescence

measurements (figure 33).

Curve

<Plate Layout Settings>

Lu

m

0 10 20 30 40 50 60

300000

400000

500000

600000

700000

800000

900000

1000000

1100000

Concentration [nM]

Re

lati

ve li

ghtu

nit

s(R

LU)

Figure 33. Concentration curve of a DiFi potency assay, detected by luminescence read-out. An exemplary, resulting concentration curve is shown by using a concentration range of 5- 55nM. Blue points indicate the individual results, orange points the mean values of the triplicates.

As a consequence, the concentration range was adapted to 0.5 – 16.7nM, for both, luminescence

and fluorescence (see figure 34).

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Curve

<Plate Layout Settings>

53

0/2

5,6

00

/40

0,01 0,1 1 10 100

50000

100000

150000

200000

250000

300000

350000

400000

Concentration [nM]

Re

lati

ve li

ghtu

nit

s(R

LU)

Figure 34. Concentration curve of a DiFi potency assay, detected by luminescence read-out.

An exemplary, resulting concentration curve is shown by using a concentration range of 0.5- 16.7nM. Blue points indicate the individual results, orange points the mean values of the triplicates.

Thus, again, the higher sensitivity of the Alamar Blue and ATP assays in comparison to the MTS

assay could be demonstrated. Similar to the CTLL-2 assay, approx. ten times lower antibody

concentrations could be detected: 0.5nM in contrast to 5nM. For the luminescence system, the cell

density used originally for the MTS read-out could be reduced from 5*105 cells/mL to 2.5*10

5

cells/mL and for the fluorescence system it could even be reduced to 1*105 cells/mL.

The incubation time with substrate was again the shortest for the luminescence read-out (5 -

10min), followed by the colorimetric system (75 15min) and the fluorescence read-out (4 0.5h).

In comparison to the CTLL-2 assay, however, the difference between the ATP and Alamar Blue

assay was not that significant since the difference by using the fluorescence technique consisted of

4h only as opposed to a whole day.

In contrast to the CTLL-2 assay only slight differences were observed between the different read-

outs regarding the signal to noise ratios. The calculated mean ratios of 2.2 for MTS, 3.0 for ATP

and 1.8 for Alamar Blue were all relatively low.

In line with the CTLL-2 assay, three repetitions of the assay on different days were performed on

the different concentration levels of 50%, 100% and 150% for all three read-outs (n = 9). Results

are summarized in tables 16 to 18.

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Table 16. Results qualification DiFi assay: expected activity 50% (i.e. relative potency: 0.5).

Read-out Colorimetric Luminescence Fluorescence

Result day 1 0.373 0.412 0.459

Result day 2 0.538 0.562 0.464

Result day 3 0.571 0.505 0.461

Mean 0.494 0.493 0.461

Recovery [%] 98.8 98.6 92.3

RE [%] 15.7 10.3 7.7

CV [%] 21.5 15.4 0.5

Table 17. Results qualification DiFi assay: expected activity 100% (i.e. relative potency: 1.0).

Read-out Colorimetric Luminescence Fluorescence

Result day 1 0.972 1.031 0.980

Result day 2 0.965 0.936 1.012

Result day 3 0.996 1.013 1.022

Mean 0.978 0.993 1.005

Recovery [%] 97.8 99.3 100.5

RE [%] 2.2 3.6 1.8

CV [%] 1.7 5.1 2.2

Table 18. Results qualification DiFi assay: expected activity 150% (i.e. relative potency: 1.5).

Read-out Colorimetric Luminescence Fluorescence

Result day 1 1.399 1.542 1.417

Result day 2 1.402 1.515 1.462

Result day 3 1.531 1.441 1.570

Mean 1.444 1.499 1.483

Recovery [%] 96.3 100.0 98.9

RE [%] 5.1 2.6 4.2

CV [%] 5.2 3.5 5.3

Recoveries including all results of the different concentration levels of 50%, 100% and 150% varied

between 74.6% and 114.2% for the colorimetric read-out, 82.4% and 112.4% for luminescence and

91.8% and 104.7% for fluorescence. Despite the lower signal to noise ratios in comparison to the

CTLL-2 assay, results of the DiFi assay were more accurate and precise. Thus, mean REs (mean

deviations from the expected activity) of 7.7%, 5.5% and 4.6% and mean CVs of 6.6%, 6.0% and

3.4% were calculated for the colorimetric, luminescence and fluorescence system, respectively.

Consequently, no major differences between the three read-outs were observed for the DiFi assay

regarding accuracy and precision.

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An overall summary of the most important parameters of the DiFi potency assay and a comparison

between the different read-outs is shown in table 19.

Table 19. Summary of DiFi assay parameters and comparison between the different read-out systems.

2.2.4. Kit 225 potency assay

In general, for the Kit 225 potency assay, the same trends as for the CTLL-2 and DiFi potency

assays could be observed.

The originally used concentration range of 5.8 – 25ng/mL for the Kit 225 assay was not suitable,

neither for the MTS read-out (see figure 35), nor for fluorescence and luminescence (see figure

37).

Read-out Colorimetric Luminescence Fluorescence

Concentration range 5 – 55nM 0.5 – 16.7nM 0.5 – 16.7nM

Signal to noise ratio 2.2

(1.8 – 2.6)

3.0

(2.6 – 3.6)

1.8

(1.4 – 2.1)

Cell density 5*105 cells/mL 2.5*10

5 cells/mL 1*10

5 cells/mL

Incubation time (with

substrate) 75 15min 5 - 10min 4 0.5h

Recovery (range) 74.6% - 114.2% 82.4% - 112.4% 91.8% - 104.7%

Accuracy

(mean RE; n = 9) 7.7% 5.5% 4.6%

Precision

(Mean CV; n = 9) 6.6% 6.0% 3.4%

Costs/plate (substrate

only) Luminescence > Fluorescence > Colorimetric

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0

0,2

0,4

0,6

0,8

1

1,2

1,4

1 10 100

y

x

Standard Curve

Concentration [ng/mL]

OD

val

ue

sat

49

0nm

Figure 35. Concentration curve of a Kit 225 potency assay, detected by colorimetric read-out. An exemplary, resulting concentration curve is shown by using a concentration range of 5.8 - 25ng/mL. Green points indicate the individual results, red points the mean values of the triplicates.

Thus, the concentration range for the colorimetric read-out was adapted to 0.35 – 40ng/mL (see

figure 36).

0

0,1

0,2

0,3

0,4

0,5

0,6

0,7

0,8

0,9

1

0,1 1 10 100

y

x

Standard Curve

Concentration [ng/mL]

OD

val

ue

sat

49

0nm

Figure 36. Optimized curve of a Kit 225 potency assay, detected by colorimetric read-out. An exemplary, resulting concentration curve is shown by using a concentration range of 0.35 - 40ng/mL. Green points indicate the individual results, red points the mean values of the triplicates.

For luminescence and fluorescence the curve shown in figure 37, was obtained by using the

original concentration range of 5.8 – 25ng/mL.

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Curve

<Plate Layout Settings>

Lu

m

1 10 100

1200000

1300000

1400000

1500000

1600000

1700000

1800000

1900000

2000000

2100000

2200000

2300000

Concentration [ng/mL]

Re

lati

ve li

ghtu

nit

s(R

LU)

Figure 37. Concentration curve of a Kit 225 potency assay, detected by luminescence read-out. An exemplary, resulting concentration curve is shown by using a concentration range of 5.8 - 25ng/mL. Blue points indicate the individual results, orange points the mean values of the triplicates.

Since this range was again not adequate, it was adapted to 0.025 – 40ng/mL, for both,

luminescence and fluorescence, resulting in the curve shown in figure 38.

Curve

<Plate Layout Settings>

53

0/2

5,6

00

/40

0,001 0,01 0,1 1 10 100

200000

400000

600000

800000

1000000

1200000

1400000

1600000

1800000

Concentration [ng/mL]

Re

lati

ve li

ghtu

nit

s(R

LU)

Figure 38. Optimized curve of a Kit 225 potency assay, detected by luminescence read-out.

An exemplary, resulting concentration curve is shown by using a concentration range of 0.025 - 40ng/mL. Blue points indicate the individual results, orange points the mean values of the triplicates.

It can be concluded, that the higher sensitivity of the luminescence and fluorescence read-outs

could again be highlighted since they detected drug concentrations of 0.025ng/mL in contrast to

0.35ng/mL detected by the colorimetric system.

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The cell density for luminescence and fluorescence could even be reduced to a tenth of the original

density of 100.000 cells/well. Furthermore, the cell suspension volume could be reduced from

70µL/well to 50µL/well. This led to significant reductions of costs and resources for cell culture

when using the Alamar Blue or ATP assays instead of the MTS assay.

Luminescence with an incubation time with substrate of 5 - 10min was again the fastest method. In

contrast, the colorimetric and fluorescence systems needed incubation times of 3 – 4h and 6 1h,

respectively.

The mean signal to noise ratios were 2.5 for MTS, 4.9 for ATP and 3.9 for Alamar Blue.

Consequently, higher ratios were observed for fluorescence and especially for luminescence than

for the colorimetric system, like for the CTLL-2 assay, even if differences were not that significant in

this case.

Subsequently, the Kit 225 assay was equally qualified with respect to accuracy and precision.

Results of the different concentration levels of 50%, 100% and 150% are summarized in tables 20

to 22.

Table 20. Results qualification Kit 225 assay: expected activity 50% (i.e. relative potency: 0.5).

Read-out Colorimetric Luminescence Fluorescence

Result day 1 0.711 0.412 0.514

Result day 2 0.449 0.487 0.405

Result day 3 0.443 0.462 0.561

Mean 0.534 0.454 0.493

Recovery [%] 106.9 90.7 98.7

RE [%] 21.3 9.3 11.3

CV [%] 28.6 8.4 16.2

Table 21. Results qualification Kit 225 assay: expected activity 100% (i.e. relative potency: 1.0).

Read-out Colorimetric Luminescence Fluorescence

Result day 1 0.979 0.951 1.013

Result day 2 1.008 1.024 0.971

Result day 3 1.117 0.985 0.971

Mean 1.035 0.987 0.985

Recovery [%] 103.5 98.7 98.5

RE [%] 4.9 3.0 3.0

CV [%] 7.0 3.7 2.5

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Table 22. Results qualification Kit 225 assay: expected activity 150% (i.e. relative potency: 1.5).

Read-out Colorimetric Luminescence Fluorescence

Result day 1 1.467 1.585 1.634

Result day 2 1.373 1.546 1.476

Result day 3 1.522 1.358 1.432

Mean 1.454 1.496 1.514

Recovery [%] 96.9 99.8 100.9

RE [%] 4.0 6.1 5.0

CV [%] 5.2 8.1 7.0

During assay qualification, recoveries including all results of all three concentration levels varied

between 88.6% and 124.2% for the colorimetric, 82.4% and 105.7% for the luminescence and

81.0% and 108.9% for the fluorescence system.

Regarding accuracy, no major differences were observed for the different read-outs since mean

REs of 10.1%, 6.1% and 6.4% were calculated for the MTS, ATP and Alamar Blue assays,

respectively.

Luminescence and fluorescence techniques had mean CVs of 6.5% and 7.0% and therefore

seemed a bit more precise than the colorimetric system showing 10.0%. The higher precision is in

good agreement with the higher signal to noise ratios and has already been observed for the CTLL-

2 potency assay.

An overall summary of the most important parameters of the Kit 225 potency assay and a

comparison between the different read-outs is shown in table 23.

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Table 23. Summary of Kit 225 assay parameters and comparison between the different read-out systems.

2.3. Combined discussion of CTLL-2, DiFi and Kit 225 assay results

As already described in the Introduction section I.3.3., assays used for QC, release and stability

testing should be precise, robust, accurate and should show a good repeatability. To accomplish

this and to be suitable for routine use in a QC environment, they should provide a high signal to

noise ratio and a stable read-out for more than 30min. Furthermore, they should be as fast as

possible; kinetic measurements are usually not used for QC.

In this regard, the three different proliferation assays used in this study were compared to each

other, considering the above mentioned parameters.

Regarding the results of all three potency assays, no major differences regarding accuracy and

precision between the different read-outs were observed. The similarity of the results of different

substrates has already been observed by Mueller et al. (2004) who compared MTT, ATP and

calcein assays and found a high correlation between them. In this study, all three read-outs

provided accurate and reproducible results. Consequently, they are all suitable for use in QC.

Workload and hands-on time were the same for all three assays. Nevertheless, the different read-

out techniques possess some advantages and disadvantages.

From the results of this study, it is clear that the luminescence and fluorescence techniques are

more sensitive than the colorimetric read-out. They could detect approx. ten times lower drug

concentrations and the assay could be performed using considerably lower cell numbers. The

higher sensitivity of the ATP assay in comparison to a colorimetric system has already been

observed by Petty et al. (1995). By comparing the sensitivity of MTT- and ATP-based assays using

Read-out Colorimetric Luminescence Fluorescence

Concentration range 0.35 – 40ng/mL 0.025 – 40ng/mL 0.025 – 40ng/mL

Signal to noise ratio, mean

(range)

2.5

(2.2 – 2.7)

4.9

(3.5 – 6.3)

3.9

(3.2 – 4.8)

Cell density 100.000 cells/well 10.000 cells/well 10.000 cells/well

Volume of API and cells 70 L/well 50 L/well 50 L/well

Incubation time (with

substrate) 3 – 4h 5 - 10min 6 1h

Recovery (range) 88.6% - 124.2% 82.4% - 105.7% 81.0% - 108.9%

Accuracy

(mean RE [%]; n = 9) 10.1% 6.1% 6.4%

Precision

(Mean CV [%]; n = 9) 10.0% 6.5% 7.0%

Costs/plate (substrate

only) Luminescence > Fluorescence > Colorimetric

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Daudi and CCRF-CEM cell lines, they found a detection limit of the luminescence method of

approx. 1.500 cells/well in contrast to 25.000 cells/well for the colorimetric system. Comparable

observations that confirm the higher sensitivity of the ATP assay were made by Eirheim et al.

(2004), Ulukaya et al. (2008), Couch and Slater (2001) and Weyermann et al. (2005). The higher

sensitivity of Alamar Blue in comparison to the MTT reagent has already been shown as well, e.g.

by Hamid et al. (2004), who compared the two reagents for high throughput screening using 117

different drugs.

Apart from the higher sensitivity of the luminescence and fluorescence techniques in comparison to

the colorimetric system, the ATP and Alamar Blue assays possess another advantage: Their signal

to noise ratios are higher. Differences between the ratios depend on the different cell lines. Nearly

the same ratios for all three read-outs were observed using the DiFi potency assay, in contrast,

approx. 3 times higher ratios were calculated for fluorescence in comparison to the colorimetric

system and approx. 5 - 6 times higher ratios were obtained for luminescence using the CTLL-2

potency assay.

The results of this study suggest that the signal to noise ratios tend to be highest for luminescence

and the lowest for the colorimetric system. In cases of a higher signal to noise ratio, this seemed to

result in a higher precision of the assay. Thus, mean CVs of 13.6% and 10.0% were obtained using

the MTS reagent for the CTLL-2 and Kit 225 assays, respectively, whereas the Alamar Blue assay

provided CVs of 6.9% and 7.0%, respectively and the ATP assay CVs of 4.3% and 6.5%,

respectively.

So far, the luminescence and fluorescence read-outs seem to be equivalent and slightly superior to

the colorimetric system for use in QC. Squatrito et al. (1995) compared Alamar Blue and ATP

bioluminescence assays for cytotoxicity screening assays and only found a poor correlation

between them with a clear recommendation for the ATP assay. In contrast, this study showed that

both read-outs are suited excellently for potency assays in QC. There were hardly any differences

in the calculated potencies and both assays are extremely sensitive. Underestimation of cytotoxic

effects using the Alamar Blue assay (Squatrito et al., 1995) is not of relevance in case of potency

assays since the sample is directly compared to a reference standard on the same 96 well plate.

Nevertheless, the fluorescence technique is less convenient in comparison to the luminescence

read-out due to its longer incubation time with substrate. The incubation times varied significantly

between the different potency assays. This is due to the fact that each cell line has unique

metabolic properties and has to be characterized individually to determine the appropriate

incubation time (Nakayama et al., 1997). The disadvantage of the longer incubation time varied in

our study between a few hours (4 - 6h) in case of the DiFi and Kit 225 assays to a whole day (24h)

in case of the CTLL-2 potency assay.

Reasons for the longer incubation times of Alamar Blue are its low toxicity and non-destructive

effect on cells. Especially for performing kinetic measurements of the changes in cell proliferation

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and viability this is of great advantage (Pagé et al., 1993; Zhi-Jun et al., 1997). In contrast to most

other reagents including the MTS and ATP read-outs, Alamar Blue does not require lysis of cells.

Thus, kinetic measurements as well as further immunological studies of the cells are possible.

However, this is of less importance in QC. Here, the longer incubation time is a disadvantage in

comparison to the colorimetric and especially the luminescence technique that require shorter

incubation times.

Finally, the only disadvantage of the luminescence technique observed in this study has to be

mentioned. The costs for the CellTiter- Glo® reagent for one plate are higher as those for the MTS

reagent and also as those for the Alamar Blue reagent. This effect could however at least partially

be reduced due to the lower number of cells required. As less cells need to be cultivated, the costs

for culture medium, growth factors etc. could be decreased.

2.4. Conclusions

Taken together, this study showed that all three read-out systems, the MTS/PMS assay, the

Alamar Blue assay and the ATP bioluminescence assay, are suited well for use in QC since they

produce reliable and reproducible results. Workload and hands-on time were the same for all three

assays.

From the results of this study however, it can be concluded that the luminescence technique seems

to be the most advantageous of the three read-outs for potency assays in QC. It is extremely

sensitive, therefore leading to cell savings and provides the highest signal to noise ratios, leading

to very precise results. Moreover, it is the fastest of the three methods for all assays investigated,

since the plate can already be measured 5 - 10min after addition of substrate.

It can thus be concluded that it is recommendable to replace the colorimetric read-out by the

luminescence technique.

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3. CHARACTERIZATION OF THE IL-7 SIGNAL TRANSDUCTION PATHWAYS AND SELECTION OF AN

APPROPRIATE TARGET FOR DEVELOPMENT OF AN INTRACELLULAR PHOSPHORYLATION ASSAY

In pharmaceutical QC, the potency of biopharmaceuticals is commonly assessed by using

proliferation assays. However, other assay formats like reporter gene or phosphorylation assays

are equally possible. The aim of this study was to develop an alternative intracellular

phosphorylation assay for Fc-IL7 since the originally used proliferation assay suffered from a very

long incubation time and a poor robustness.

Therefore, first of all, the IL-7 signal transduction pathways had to be screened for a suitable target

for development of a phosphorylation assay. This study was further expanded to a comparison

between different human T and murine B cell lines, as well as to a comparison between IL-2 and

IL-7 signaling. The cell lines used for this comparison were the following:

Kit 225 cells are human IL-2 dependent T lymphocytes, derived from a patient with T cell chronic

lymphocytic leukemia with OKT3+, -T4

+, - T8

– phenotype (Hori et al., 1987). Mehrotra et al. (1995)

showed that Kit 225 cells were equally proliferating in presence of IL-7.

Due to the fact that Kit 225 cells are stimulated by both, IL-2 and IL-7, they are suited well for a

comparison between those two γc cytokines.

Furthermore, two different B cell lines were used, at a different stage of maturation:

First, the pre-B cell line, PB-1, derived from bone marrow cells from CBA/C57BL mice and cloned

in the presence of IL-7 (Mire-Sluis et al., 2000); and second, the lymphocyte clone 2E8, which was

isolated from murine long-term bone marrow cultures and used for the initial selection of a series of

stromal-cell clones (Pietrangeli et al., 1988). To my knowledge, no IL-2 dependency of those two

cell lines has been published to date.

In order to elucidate the IL-7 signaling cascade, representative targets of some of the most

important pathways, presumed to be activated by IL-7, were selected. In comparison to other

cytokines, relatively little is known about the IL-7 pathways. Some pathways which are presumed to

be activated by IL-7, and consequently were investigated in this study are the JAK/STAT, the

PI3K/AKT, the ERK, the SFK and the p38MAPK pathways. They are described in detail in the

Introduction section I.2.3.

The pathways were studied in three different cell lines (Kit 225, PB-1 and 2E8 cells) using western

blotting and the receptor densities of the different cells were measured using flow cytometric

analysis. Moreover, IL-2 and IL-7 signaling pathways were compared in Kit 225 cells. Prior to

western blotting and flow cytometric analyses, cells were starved for one day without growth factor

and were then incubated with IL-2 or IL-7 for various times at 37°C as described under Materials

and Methods. Experiments were performed at least in duplicates starting from activation of the

cells. One representative example is shown. The correct bands in the western blotting analyses

were identified with the help of a positive control and the denoted molecular weight of the

respective protein.

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3.1. Results and Discussion of flow cytometric analyses

In order to compare the IL-2R and IL-7R densities of the different cell lines, flow cytometric

analyses were performed on the three cell lines. IL-7R was present on all three cell lines (see

figure 39). However, expression was relatively low on Kit 225 cells, where the increase in

fluorescence intensity was smaller than 1 log. The highest IL-7R expression was noticed for 2E8

cells.

Figure 39. Flow cytometric analysis of IL-7Rα densities on A) Kit 225, B) PB-1, and C) 2E8 cells.

In figure 39D, all histograms of the different cell lines were overlaid in order to compare the receptor densities of the different cell lines to each other. Cells were either labeled with isotype controls (red histogram) or CD127 antibodies (green histogram), both PE conjugated. IL-7Rα was present on all cell lines; the density was the lowest on Kit 225 cells and the highest on 2E8 cells. The shown histograms are representatives of two independent experiments.

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As expected, IL-2R density was much higher than IL-7R density on Kit 225 cells. Surprisingly,

this was the same for PB-1 and 2E8 cells, even if the increase in fluorescence intensity was

smaller than for Kit 225 cells (see figure 40).

Figure 40. Flow cytometric analysis of IL-2Rα densities on A) Kit 225, B) PB-1, and C) 2E8 cells. In figure 40D, all histograms of the different cell lines were overlaid in order to compare the receptor densities of the different cell lines to each other. Cells were either labeled with isotype controls (red histogram) or CD127 antibodies (green histogram), both PE conjugated. IL-2Rα was present on all cell lines; the density was the lowest on PB-1 cells and the highest on Kit 225 cells. The shown histograms are representatives of two independent experiments.

CD25 and thus IL-2R expression has already been described for PB-1 cells (Mire-Sluis, 2000);

nevertheless no IL-2 dependency has been reported neither for them, nor for the 2E8 cells.

Consequently, in addition, the IL-2R densities were analyzed on the different cell lines. IL-2R is

the part of the receptor, which is presumed to be responsible for signal transduction (Minami et al.,

1993). It could be clearly shown that IL-2R is not expressed on PB-1 and 2E8 cells, but on Kit 225

cells (see figure 41).

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Figure 41. Flow cytometric analysis of IL-2Rβ densities on A) Kit 225, B) PB-1, and C) 2E8 cells.

In figure 43D, all histograms of the different cell lines were overlaid in order to compare the receptor densities of the different cell lines to each other. Cells were either labeled with isotype controls (red histogram) or CD127 antibodies (green histogram), both PE conjugated. IL-2Rβ was present only on Kit 225 cells; not on PB-1 and 2E8 cells. The shown histograms are representatives of two independent experiments.

From the results of the flow cytometric analyses, IL-7 induced signal transduction pathways can be

expected in all three cell lines. IL-2 induced pathways should be activated in Kit 225 cells only;

even to a stronger extent than IL-7 induced pathways due to the higher density of IL-2Rα in

comparison to IL-7Rα. In general, no IL-2 mediated pathways would be expected in PB-1 and 2E8

cells, even if they express the IL-2Rα chain. However, they do not express the -chain of the IL-2R.

A whole IL-2R, consisting of α-, β-, and γ-chain is necessary for signal transduction. Moreover, the

β-chain is the part of the receptor, which is presumed to be responsible for signal transduction.

This is in line with literature results since no IL-2 dependency has been published for these two cell

lines. It might be possible, that those differences in the expression pattern of the different receptors

are due to the difference between murine (PB-1 and 2E8) and human (Kit 225) cell lines. This is

possible; however, it has been described in literature that the receptors are highly homologous, e.g.

the human and murine IL-7R shows a homology of 64% (Goodwin et al., 1990). All six extracellular

and four intracellular cystein residues are conserved in both receptor molecules. Consequently the

possibility is rather low that the differences in the receptor expression are species dependent.

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3.2. Results and Discussion of western blotting analyses

3.2.1. Representative targets of the JAK/STAT pathway: STAT1, STAT3, STAT5, pim-1 and bcl-2

The JAK/STAT pathway is the first pathway, which is induced upon receptor activation. After JAK1

and JAK3 are activated, STATs bind to the receptor and become tyrosine phosphorylated. STAT1,

STAT3 and STAT5 were selected as examples of these pathways, in order to see, whether these

molecules were activated upon IL-7 and/or IL-2 stimulation.

3.2.1.1. STAT1 and STAT3

In this study, no phosphorylation of STAT1 (Tyr701) and STAT3 (Tyr705) were found upon IL-7

stimulation in all three cell lines, although unphosphorylated STAT molecules were present in the

cells. In contrast, both molecules were activated by IL-2 in Kit 225 cells, even if signals were very

weak (see figures 42 and 43).

STAT1 p-STAT1

kDa

250

98

64

50

36

16kDa

250

98

64

50

36

16

Figure 42. Western blotting analysis of STAT1 and phospho (p)-STAT1 in Kit 225, PB-1 and 2E8 cells. Cells were either incubated 10min at 37°C with 100ng/mL IL-7 or IL-2 or used untreated, followed by immunoblotting with anti-STAT1 and anti-phospho STAT1 antibodies as described under Materials and Methods. The figure shows that STAT1 phosphorylation (MW ≈ 85kDa) is only induced by IL-2 in Kit 225 cells. Lysates from HT29 cells incubated with interferon α served as a positive control; untreated Kit 225 cells as a negative control. The blots were developed using IR fluorescence and are one selected representative of three independent experiments.

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STAT3 p-STAT3

kDa

250

98

64

50

36

16

kDa

180

26

4937

115

82

Figure 43. Western blotting analysis of STAT3 and phospho-STAT3 in Kit 225, PB-1 and 2E8 cells. Cells were either incubated 10min at 37°C with 100ng/mL IL-7 or IL-2 or used untreated, followed by immunoblotting with anti-STAT3 and anti-phospho STAT3 antibodies as described under Materials and Methods. The figure shows that STAT3 phosphorylation (MW ≈ 80kDa) is only induced by IL-2 in Kit 225 cells. Lysates from HT29 cells incubated with interferon α served as a positive control; untreated Kit 225 cells as a negative control.The blots were developed using IR fluorescence and are one selected representative of three independent experiments.

IL-2 mediated STAT1 and STAT3 activation in Kit 225 cells have already been shown by

Delespine-Carmagnat et al. (2000). As expected, no IL-2 mediated STAT1 and STAT3 activation

has been observed in PB-1 and 2E8 cells, emphasizing the fact that the -chain of the IL-2

receptor is responsible for signal transduction.

It is unclear, why STAT1 and 3 were not phosphorylated upon IL-7 stimulation in all three cell lines

since this has already been shown for T as well as B cells. IL-7 induced STAT1 and 3 activation

has for example been demonstrated in B cell precursor acute lymphoblastic leukemia (BCP-ALL)

cells (van der Plas et al., 1996), CD4+ naïve T cells (Li et al., 2009) and HBP T lymphoblasts

(Rosenthal et al., 1997). However, to my knowledge, STAT1 and STAT3 activation has been

observed only in primary cells, not in cell lines, so far. Moreover, it has to be mentioned that the IL-

7 induced STAT3 phosphorylation was much weaker than the IL-2 induced phosphorylation in T

lymphoblasts (Rosenthal et al., 1997). In this study, only a very weak signal was obtained for

STAT3 phosphorylation in Kit 225 cells upon IL-2 stimulation, already suggesting that no or only

very slight signals could be obtained upon IL-7 stimulation, due to the lower IL-7 receptor densities.

Culture conditions in this study were similar to those of Rosenthal et al. (1997), who also starved

the cells from IL-2 containing medium for 16 – 48h prior to restimulation with IL-2 or IL-7, making

the two studies comparable.

In conclusion, STAT1 and STAT3 activation seem not to occur upon IL-7 stimulation in all three cell

lines investigated and only play a minor role in Kit 225 cells treated with IL-2.

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3.2.1.2. STAT5

In contrast to STAT1 and 3, it could be demonstrated that STAT5 was phosphorylated at Tyr694 by

IL-7 in all three cell lines after 10min incubation at 37°C (see figure 44).

STAT5 p-STAT5

kDa

98

64

50

36

16

kDa

16

50

36

250

98

64

Figure 44. Western blotting analysis of STAT5 and phospho-STAT5 in Kit 225, PB-1 and 2E8 cells.

Cells were either incubated 10min at 37°C with 100ng/mL IL-7 or IL-2 or used untreated, followed by immunoblotting with anti-STAT5 and anti-phospho STAT5 antibodies as described under Materials and Methods. The figure shows that STAT5 phosphorylation (MW ≈ 90kDa) is induced by IL-7 in all three cell lines and by IL-2 in Kit 225 cells only. In these cells, IL-2 induced phosphorylation is much stronger than IL-7 induced phosphorylation. Lysates from Hela cells incubated with interferon α served as a positive control (pos. C.); untreated Kit 225 cells as a negative control (neg. C.).The blots were developed using IR fluorescence and are one selected representative of at least five independent experiments.

The results are in line with previous observations describing IL-7 induced STAT5 phosphorylation

in several different cells, e.g. in CD34+ thymocytes (Pallard et al., 1999), primary human T and NK

cells (Yu et al., 1998), CT6 cells (Foxwell et al., 1995), HEK293T, CHO and COS-7 cells (Toda et

al., 2008), as well as in PB-1 cells (Hirokawa et al., 2003). To my knowledge, this has not yet been

published for IL-7 induced STAT5 phosphorylation in 2E8 and Kit 225 cells. Interestingly, the two

distinct bands of the different isoforms, STAT5A and STAT5B could clearly be identified in Kit 225

cells, whereas only one single band could be detected in PB-1 and 2E8 cells. This might lead to the

conclusion that only one isoform is activated in PB-1 and 2E8 cells, which is most probably

STAT5A (due to the higher molecular weight of this band; see Delespine-Carmagnat et al., 2000).

This isoform is activated in a stronger way in Kit 225 cells, too.

Like IL-7, IL-2 equally induced STAT5 activation in Kit 225 cells, showing even a much stronger

signal than IL-7. This is in good agreement with the stronger STAT3 phosphorylation by IL-2 in T

lymphoblasts in comparison to IL-7, shown by Rosenthal et al. (1997), already discussed, and the

higher IL-2R densities in comparison to IL-7R, observed in this study.

In general, IL-2 induced STAT5 phosphorylation was much stronger than IL-2 induced STAT1 and

STAT3 activation. The same phenomen has already been shown in Kit 225 cells by Delespine-

Carmagnat et al. (2000) using western blotting and electrophoretic mobility shift assay (EMSA).

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The culture conditions for the Kit 225 cells were comparable; however Carmagnat et al. (2000)

utilized antibiotic supplemented medium and starved the stells for 48h instead of 24h. IL-7

mediated effects in Kit 225 cells have not been investigated by them.

From the results discussed above, it can be concluded, that STAT5 is probably more important

than the other STATs in IL-2 and IL-7 signaling.

In order to further explore this pathway and to compare the different cell lines, additional kinetic

measurements were performed (see figure 45). Therefore, incubation times of 10min, 30min, 1h,

3h, 6h, 18h and 24h were used with IL-2 and IL-7, respectively.

Kit 225

+ IL-2

PB-1

+ IL-7

2E8

+ IL-7

Kit 225

+ IL-7

C

10

min

30

min 1h 3h 6h 18h 24h

kDa

90

90

90

90

Figure 45. Kinetic measurements of STAT5 phosphorylation.

Cells were incubated with IL-7 and IL-2 for the indicated time points between 10min and 24h. Differences in kinetics were observed between the different cell lines. The blots were developed using IR fluorescence and are one selected representative of two independent experiments.

In Kit 225 cells, a relatively stable signal for STAT5 was obtained between 10min and 6h with a

maximum after 30min, which decreased after longer incubation times (18h and 24h), for both, IL-2

and IL-7. In contrast, in 2E8 and PB-1 cells, only a weak signal (especially for PB-1) was noticed

after 10min incubation time, which then increased and remained approximately constant up to at

least 24h (experiment was completed after 24h – longer incubation times were not tested). This

difference might be explained by the different manners in which IL-7 reacts in the different cell

types. Apparently, STAT5 phosphorylation is faster induced in T than in B cells in this study;

however the signal is more stable in B cells.

3.2.1.3. Inhibition of STAT5 by WP1066

In order to clarify whether STAT5-phosphorylation could be inhibited, and thus to verify that STAT5

was really activated upon IL-7 stimulation, the JAK2/STAT3 inhibitor WP1066 was used. WP1066

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is a novel, more potent AG490 analogue (Iwamaru et al., 2007). It has been observed that WP1066

inhibited JAK2 and its downstream STAT and PI3K pathways and induced caspase-dependent

apoptosis of acute myeloid leukemia (AML) cells (Ferrajoli et al., 2007). Moreover, it activated Bax,

suppressed the expression of c-myc, bcl-xL and mcl-1, and induced apoptosis (Iwamaru et al.,

2007).

Since some STATs share the same regulatory pathway, WP1066 is supposed not only to inhibit

STAT3, but also STAT5 phosphorylation. This has already been observed in OCIM2 and K562

cells (Ferrajoli et al., 2007), as well as in U87-MG cells (Iwamaru et al., 2007); in contrast STAT5

phosphorylation was not inhibited by WP1066 in U373-MG cells.

In order to test whether STAT5 phosphorylation could be inhibited in our cell lines by WP1066, the

cells were incubated with 10µM WP1066 for 24h prior to stimulation with IL-2 or IL-7. Cells were

then subjected to western blot analysis and incubated with anti-phospho-STAT5 antibody as

described under Materials and Methods.

In this study, STAT5 phosphorylation was inhibited by WP1066 in Kit 225 and 2E8 cells, but not in

PB-1 cells upon the given conditions (see figure 46). Thus, it can be concluded, that WP1066

reacts differently in the different cell lines, which is in line with the observation made by Iwamaru et

al. (2007) who found differences between U87-MG and U373-MG cells.

kDa

98

64

50

36

16

Inhibition of p-STAT5 with WP1066

Figure 46. Inhibition of STAT5 phosphorylation by WP1066. Prior to stimulation with IL-2 or IL-7, cells were incubated with 10µM WP1066 for 24h, as described under Material and Methods. WP1066 inhibits STAT5 phosphorylation in Kit 225 cells and 2E8 cells; but not in PB-1 cells. The blots were developed using IR fluorescence and are one selected representative of two independent experiments.

The selected conditions, 10µM WP1066 and 24h, should ensure an inhibitory effect according to

other publications, already mentioned. Iwamaru et al. (2007) observed an inhibitory effect of

WP1066 between 5h and 24h using 10µM WP1066, whereas Ferrajoli et al. (2007) already noticed

his effectt after 2h using 2µM WP1066. Nevertheless, longer incubation times with higher

concentrations of WP1066 were tested in PB-1 cells, in order to check whether an inhibitory effect

could be seen. Therefore, extreme conditions using 100µM for 24h, 10µM for 48h and 100µM for

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48h were used. However, viability of PB-1 cells was strongly decreased upon these conditions

allowing no proper analysis since the protein content decreased too much in comparison to the

untreated sample.

It can be concluded, that WP1066 reacted differently in the three cell lines according to standard

conditions reported in the literature. This might be explained by the differences between the three

cell lines as well as by a lacking specificity of WP1066.

3.2.1.4. Pim-1

It has been reported that STAT5 can bind directly to the pim-1 promoter at the ISFR/GAS-

sequence, leading to an up-regulated expression of the serine/threonine kinase pim-1. Pim-1 itself

can negatively regulate the JAK/STAT pathway by binding to suppressor of SOCS proteins, a

group of negative regulators of STAT activity (Losmann et al., 1999).

IL-7 induced pim-1 up-regulation has already been detected using gene array analysis in D1 cells

after 2h incubation with IL-7 (Kim et al., 2003). Furthermore, increased mRNA expression of pim-1

upon IL-7 stimulation has been observed in TSH119 cells (Sato et al., 2001) and pro-B cells (Goetz

et al., 2004).

It should thus be investigated, whether an up-regulated expression of pim-1 and an inhibitory effect

of STAT5 phosphorylation could be found in the cell lines used.

After 10min incubation time, no pim-1 kinase was expressed in all three cell lines (see figure 47).

Pim-1

kDa

64

50

36

16

98

250

Figure 47. Western blotting analysis of pim-1 in Kit 225, PB-1 and 2E8 cells. Cells were either incubated 10min at 37°C with 100ng/mL IL-7 or IL-2 or used untreated, followed by immunoblotting with anti-pim-1 antibody as described under Materials and Methods. The figure shows that pim-1 (MW ≈ 33kDa) is not expressed in all three cell lines after 10min incubation with IL-2 or IL-7. Lysates from K562 cells served as a pos. C.; untreated Kit 225 cells as a neg. C. The blots were developed using IR fluorescence and are one selected representative of three independent experiments.

However, pim-1 was up-regulated upon longer incubation times with IL-2 and Il-7 (see figure 48).

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Kit 225

+ IL-2

PB-1

+ IL-7

2E8

+ IL-7

Kit 225

+ IL-7

C

10

min

30

min 1h 3h 6h 18h 24h

kDa

33

33

33

33

Figure 48. Kinetic measurements of pim-1 up-regulation.

Cells were incubated with 100ng/mL IL-7 and IL-2 for the indicated time points between 10min and 24h. Pim-1 was up-regulated in all three cell lines; however differences in kinetics were observed between the different cell lines. The blots were developed using IR fluorescence and are one selected representative of two independent experiments.

In Kit 225 cells, pim-1 was detected after 3h and 6h incubation time, after longer incubation times

(18h and 24h) only a very weak signal remained. This was the same for IL-2 and IL-7 stimulated

cells; however, signals were again much weaker upon IL-7 stimulation. In 2E8 and PB-1 cells, the

pim-1 kinase could already be detected after 30min and 10min incubation with IL-7, respectively.

(In PB-1 cells, a slight pim-1 expression could already be noticed in the untreated control in the

kinetic experiment.) The signal increased up to 3h and 1h, respectively, and then remained

constant for both cell lines up to 24h. Consequently, again, differences between B and T cells were

observed.

However, in both cases, no inhibitory effect on STAT5 phosphorylation could be detected. In case

of the Kit 225 cells, both STAT5 and pim-1 decreased upon longer incubation times (18h, 24h); in

contrast, the signals remained constant in 2E8 and PB-1 cells.

In general, IL-7 induced phosphorylation of STAT5 and up-regulation of pim-1 was always stronger

in PB-1 and in 2E8 cells than in Kit 225 cells, which was in good agreement with the results of the

flow cytometric analyses, showing lower IL-7R densities of the Kit 225 cells in comparison to the

other two cell lines.

3.2.1.5. Bcl-2

After phosphorylation, STAT5 induces a downstream cascade, e.g. it dimerizes and translocates to

the nucleus where it exerts its effect on transcription of regulated target genes. One possible

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downstream target of STAT5 are members of the bcl-2 family (Debierre-Grockiego, 2004). Bcl-2 is

a potent anti-apoptotic protein, which improves survival of T lymphocytes (Strasser et al., 1996).

Since STAT5 phosphorylation was observed in all three cell lines, it could be supposed that IL-7

mediated bcl-2 up-regulation could be detected in the cell lines investigated. This has for example

already been reported for D1 cells (Kim et al., 2003), immature thymocytes (von Freeden-Jeffry et

al., 1997) and human T lymphocytes (Amos et al., 1998).

However, no bcl-2 expression was found in Kit 225 cells. In contrast, bcl-2 was expressed in 2E8

and PB-1 cells (see figure 49). Consequently, differences in the expression pattern could be seen

between T and B cells. Indeed, there was no difference between treated and untreated PB-1 and

2E8 cells. No up-regulation of bcl-2 could be detected within 6h incubation time with IL-7 (data not

shown). Thus, according to this data, the bcl-2 pathway was not specifically induced by IL-7 in all

three cell lines investigated.

Bcl-2

kDa

64

50

36

16

98

250

Figure 49. Western blotting analysis of bcl-2 in Kit 225, PB-1 and 2E8 cells. Cells were either incubated 10min at 37°C with 100ng/mL IL-7 or IL-2 or used untreated, followed by immunoblotting with anti-bcl-2 antibody as described under Materials and Methods. The figure shows that bcl-2 (MW ≈ 28kDa) was expressed in PB-1 and 2E8 cells only; and not in Kit 225 cells. Lysates from Jurkat, cells served as a pos. C., untreated Kit 225 cells as a neg. C. The blots were developed using IR fluorescence and are one selected representative of three independent experiments.

A possible reason, why no up-regulation of bcl-2 was found, might be the fact that the starvation

time without IL-7 of 24h was too long since it has been described that bcl-2 levels rapidly declined

already after 2-3h (Kim et al., 2003). Moreover, IL-7 does not necessarily enhance bcl-2

expression, but only protects cells from a decline in bcl-2, as it has already been observed in T

cells (Kim et al., 1998; Hernández-Caselles et al., 1995) and 103 cells (Banerjee and Rothman,

1998). Thus, in Kit 225 cells, supposably no up-regulation could be detected since no bcl-2 was

expressed or has already completely disappeared due to the too long incubation time. In PB-1 and

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2E8 cells probably only a preserving but no stimulating effect of IL-7 could be observed. In line with

this, no significant changes in bcl-2 expression in neither 697neo nor 697D5A4 cells were observed

upon IL-7 stimulation (Lavin et al., 2004).

Moreover, it has been reported that PI3K activation was mandatory for IL-7–mediated bcl-2 up-

regulation (Barata et al., 2004), and no IL-7 induced AKT (and consequently presumably no PI3K

activation) was observed in the cell lines investigated, which will be discussed in the following.

3.2.2. Representative target of the PI3K/AKT pathway: AKT

Another kinase, which is supposed to be activated upon IL-7 stimulation, is PI3K. Their p85 subunit

binds to the phosphorylated Y449 residue on the IL-7R chain via an SH domain and activates

subsequently the catalytic subunit. The major effector of PI3K signaling is the serine/threonine

kinase AKT, which was selected as a representative target of this pathway.

In this study, no IL-7 mediated AKT activation was detected in all three cell lines investigated. In

contrast, AKT was phosphorylated at Ser473 upon IL-2 stimulation in Kit 225 cells (see figure 50).

This has already been shown for Kit 225 cells by Avota et al. (2001), who analyzed IL-2R signaling

in primary human T cells and Kit 225 cells. As expected, no IL-2 induced AKT activation was found

in PB-1 and 2E8 cells due to the lacking -chain of the IL-2R.

AKT p-AKT

kDa

250

98

64

50

36

kDa

98

64

50

36

1616

--

Figure 50. Western blotting analysis of AKT and phosphor-AKT in Kit 225, PB-1 and 2E8 cells.

Cells were either incubated 10min at 37°C with 100ng/mL IL-7 or IL-2 or used untreated, followed by immunoblotting with anti-AKT and anti-phospho-AKT antibodyies as described under Materials and Methods. The figure shows that AKT phosphorylation (MW ≈ 60kDa) is only induced by IL-2 in Kit 225 cells. Lysates from Jurkat cells incubated with calyculin A and LY294002 served as a pos. C. and neg. C., respectively.The blots were developed using IR fluorescence and are one selected representative of three independent experiments.

Again, it remains unclear, why no IL-7 mediated AKT activation was found in the cell lines tested

since this has already been reported for D1 cells (Li et al., 2004) and T-ALL cells (Barata et al.,

2004). On the other side, it has been reported that IL-7 did not activate the PI3K pathway and did

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not phosphorylate AKT, although cells were proliferating in presence of IL-7 (Lali et al., 2004).

Moreover, Osborne et al. (2007) observed that AKT phosphorylation was only induced by IL-2, not

by IL-7 in T cells, confirming the results of this study.

Lali et al. (2004) reported that IL-2 induced two waves of PI3K activity in CT6 and F7 cells: one

rapid wave occurring within minutes and a second later wave, occurring within hours (3h – 6h),

which contributed to T cell growth. They presumed that IL-7 only induced the second, later wave of

PI3K/AKT activation. Consequently, some kinetic measurements with longer incubation times with

IL-2 and IL-7 were performed, in order to see whether this second wave was induced in our cell

lines. However, no AKT activation was found within 6h incubation time with IL-7 in all three cell

lines (see figure 51). Besides, no second wave of IL-2 mediated AKT activation was found in Kit

225 cells. Instead, the signal was stable between 10min and 30min and then decreased upon

longer incubation times.

Kit 225 stimulated with IL-2 and IL-7 2E8 and PB-1 stimulated with IL-7

kDa

250

986450

36

16

kDa

98

64

50

36

16

250

Figure 51. Kinetic measurements of AKT phosphorylation. Cells were incubated with IL-7 and IL-2 for the indicated time points between 10min and 6h. No IL-7 induced AKT phosphorylation was observed for all time points in all three cell lines; the signal for IL-2 mediated AKT phosphorylation in Kit 225 cells was stable between 10min and 30min and then decreased upon longer incubation times. The blots were developed using IR fluorescence and are one selected representative of two independent experiments.

3.2.3. Representative targets of the ERK pathway: ERK and Bim

Another pathway, which is induced by some of the c family cytokines, is the p42/44 ERK cascade,

which regulates the activity of the pro-apoptotic protein Bim and the NHE, regulating the pH of the

cell.

3.2.3.1. ERK

Like STAT1, STAT3 and AKT, ERK phosphorylation (Thr202/ Tyr204) was only induced by IL-2 in

Kit 225 cells. This has already been shown in Kit 225 cellls by Blanchard et al. (2000) and Arnaud

et al. (2004). In PB-1 and 2E8 cells, again, no IL-2 induced ERK activation was found, due to the

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lacking -chain of the IL-2R. No IL-7 induced phosphorylation was found in all three cell lines

investigated (see figure 52).

ERK p-ERK

kDa

250

98

64

50

36

kDa

250

98

64

50

36

16

16

Figure 52. Western blotting analysis of ERK and phospho-ERK in Kit 225, PB-1 and 2E8 cells. Cells were either incubated 10min at 37°C with 100ng/mL IL-7 or IL-2 or used untreated, followed by immunoblotting with anti-ERK and anti-phospho-ERK antibodyies as described under Materials and Methods. The figure shows that ERK phosphorylation (MW ≈ 42/44kDa) is only induced by IL-2 in Kit 225 cells. Lysates from Kit 225 cells incubated with FBS served as a pos. C.; untreated Kit 225 cells as a neg. C. The blots were developed using IR fluorescence and are one selected representative of three independent experiments.

Furthermore, kinetic measurements revealed no IL-7 induced phosphorylation in all three cell lines

investigated between 10min and 6h incubation time with IL-7. The signal for IL-2 induced ERK

phosphorylation was stable between 10min and 1h and then decreased upon longer incubation

times (see figure 53).

2E8 and PB-1 stimulated with IL-7

kDa

98

64

50

36

16

kDa

Kit 225 stimulated with IL-2 and IL-7

98

64

50

36

16

Figure 53. Kinetic measurements of ERK phosphorylation. Cells were incubated with IL-7 and IL-2 for the indicated time points between 10min and 6h. No IL-7 induced ERK phosphorylation was observed for all time points in all three cell lines; the signal for IL-2 mediated ERK phosphorylation in Kit 225 cells was stable between 10min and 1h and then decreased upon longer incubation

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times.The blots were developed using IR fluorescence and are one selected representative of two independent experiments.

In contrast to some of the other signal transduction pathways investigated so far, which were

supposed to be activated by IL-7, but were not induced in the cell lines investigated in this study,

results of this study are in good agreement with current literature regarding the ERK pathway.

Like for AKT, Osborne et al. (2007) observed that ERK phosphorylation was only induced by IL-2,

not by IL-7 in T cells, confirming the results of this study. According to Crawley et al. (1996), the

ERK pathway was not induced in most cell types upon IL-7 stimulation, at least not in murine T cell

lines (reviewed in Kittiparin and Khaled, 2007). In contrast to normal T cells, it has however been

shown to be activated in T-ALL cells (Barata et al., 2004) and in pre-B cells (Fleming et al., 2001).

The reason, why the ERK pathway is not activated by IL-7 in most cell lines, might be explained by

the lacking -chain of IL-7. The acidic region of the IL-2R is the docking site for Src homology and

collagen (Shc), which is the adaptor molecule for the ERK pathway. Since no ß-chain is present on

the IL-7R, Shc can bind and the signal transduction cascade can not be initiated. Similar

observations have already been made by Hsu et al. (2008), who found Shc activation by IL-2 only,

and not by IL-7 in common lymphoid progenitors (CLPs).

3.2.3.2. Bim

Bim is a pro-apoptotic member of the bcl-2 family, existing in three isoforms: BimS, BimL and BimEL

(O‟Connor et al., 1998). Bim has a role in the death of antigen-activated T cells (Snow et al., 2008)

and deficiency of Bim rescued the T cell depleted phenotype of IL-7 receptor deficient mice

(Pellegrini et al., 2004). Upon apoptotic stimuli, Bim is released from the dynein motor complex by

a mechanism including phosphorylation on T56 and S58 by JNK, leading to an increase in the

apoptotic activity (Lei et al., 2003). It is potentially regulated by IL-7 (Li et al., 2009) and can be

phosphorylated and thus inactivated by STAT5, AKT and especially ERK (Harada et al., 2004). Bim

might thus be a target of IL-7 signaling (Jiang et al., 2005). It has been observed, that IL-7

decreased the amount of Bim in T cells derived from tumor-bearing mice, which was associated

with a decrease in the apoptosis rate of these cells (Andersson et al., 2009).

According to the results of this study, however, Bim was not expressed in Kit 225 cells. In PB-1 and

2E8 cells, it was expressed but no regulatory effect of IL-7 could be observed between 10min and

6h incubation time with IL-7 (see figure 56; kinetics not shown). Thus, Bim regulation was not

specifically mediated by IL-7 in all three cell lines. This is in line with observations made by Oliver

et al. (2004), who reported that Bim was expressed in all stages of B cell maturation, but its level

was unaffected by IL.7. Comparable observations were made by Li et al. (2010), who noticed that,

even if deletion of Bim partially protected an IL-7-dependent T cell line and peripheral T cells from

IL-7 deprivation, IL-7 withdrawal did not increase Bim mRNA or protein expression but did only

induce a change in BimEL isoelectric point and reactivity with an anti-phosphoserine antibody. Li et

al. (2010) concluded that maintenance of peripheral T cells by IL-7 was partly mediated through

inhibiting Bim activity at the posttranslational level.

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The apoptotic activity of Bim and the interaction with Bax, another pro-apoptotic protein, can be

regulated by phosphorylating BimEL on three serine sites, S55, S65, and S100 (Harada et al.,

2004). It should consequently be explored, whether Bim was phosphorylated in the cell lines

investigated, by using an anti-phospho-Ser55-antibody. However, no phosphorylation of Bim was

found between 10min and 6h incubation time with IL-7 in all three cell lines (see figure 54; kinetics

not shown). This was the same for IL-2 induced phophorylation, even if both, ERK and AKT –

presumed to phosphorylate Bim - were activated upon IL-2 stimulation in Kit 225 cells.

Bim p-Bim

kDa

250

98

64

50

36

16

kDa

250

98

64

50

36

16

Figure 54. Western blotting analysis of Bim and phospho-Bim in Kit 225, PB-1 and 2E8 cells. Cells were either incubated 10min at 37°C with 100ng/mL IL-7 or IL-2 or used untreated, followed by immunoblotting with anti-Bim and anti-phospho-Bim antibodies as described under Materials and Methods. The figure shows that Bim (MW ≈ 25kDa) was expressed in PB-1 and 2E8 cells only; and not in Kit 225 cells. Lysates from HuT78 cells served as a pos. C.; untreated Kit 225 cells as a neg. C. The blots were developed using IR fluorescence and are one selected representative of three independent experiments.

3.2.4. Representative target of the SFK pathway: Lck

SFKs are non-receptor tyrosine kinases, which are supposed to be activated by IL-7 (Seckinger et

al., 1994), although none of the members yet have been shown to be uniquely required for IL-7.

SFKs include nine members, beyond them Lck, which we selected as representative target of this

family since it is one of the two most abundantly expressed SFKs in T cells (Mustelin et al., 1994).

It can be co-immunoprecipitated with the β-chain of the IL-2R indicating its association with the

receptor complex. Upon IL-7 stimulation, Lck undergoes phosphorylation (Page et al., 1995).

In this study, no Lck expression was found in Kit 225 cells. This confirms the observations of Mills

et al. (1992), who showed that Kit 225 cells are lacking Lck expression, but can nevertheless

activate JAK3. In contrast, Lck and phospho-Lck (Tyr505) were expressed in PB-1 and 2E8 cells

(see figure 55).

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Lck p-Lck

kDa

250

98

64

50

36

16kDa

250

98

64

50

36

16

Figure 55. Western blotting analysis of Lck and phospho-Lck in Kit 225, PB-1 and 2E8 cells. Cells were either incubated 10min at 37°C with 100ng/mL IL-7 or IL-2 or used untreated, followed by immunoblotting with anti-Bim and anti-phospho-Bim antibodies as described under Materials and Methods. The figure shows that Lck and p-Lck (MW ≈ 56kDa) were expressed in PB-1 and 2E8 cells only; and not in Kit 225 cells. Lysates from CCRF-HSB-2 cells served as a pos. C.; untreated Kit 225 cells as a neg. C. The blots were developed using IR fluorescence and are one selected representative of three independent experiments.

For 2E8 cells, Lck expression has already been observed by Ishihara et al. (1991). In addition to

bcl-2 and Bim, Lck is the third target, which was not expressed in Kit 225 cells, but only in the two

B cell lines, PB-1 and 2E8. Therein, clear differences in the expression pattern of T and B cells

could be identified in this study. However, these observations are in opposition to those of

Venkitaraman and Cowling (1992) who reported that phospho-Lck was predominantly T-

lymphocyte-restricted, and was only expressed at low levels in a few B lymphocyte lines. Another

possibility would be that the difference in the expression pattern is due to the difference between

human (Kit 225) and murine (PB-1 and 2E8) cell lines. However, as already reported, the human

and murine IL-7R show a high degree of homology (64%) (Goodwin et al., 1990). Moreover, all of

the three positive controls for bcl-2 (Jurkat), Bim (HuT 78) and Lck (CCRF-HSB-2) are of human

origin. Thus, those targets are in general expressed in human cell lines and failure of the antibodies

etc. can be excluded.

As for bcl-2 and Bim however, again, no difference between treated and untreated PB-1 and 2E8

cells was found. No effect of IL-7 could be seen between 10min and 6h incubation time (data not

shown). The reason for this remains unclear since IL-7 induced Lck-phosphorylation has already

been observed in T cells (Sharfe and Roifman, 1997; Page et al., 1995). Moreover, IL-7 mediated

up-regulation of Lck has been noticed in D1 cells (Kim et al., 2003). On the other hand, no increase

in phospho-Lck activity was observed in Nalm-6 cells (Seckinger et al., 1994). In this cell line, the

only member of the Src family to be stimulated by IL-7 was Fyn.

It can be concluded, that in this study, Lck was not specifically activated upon IL-7 stimulation in all

three cell lines investigated. However, it is possible that other members of the Src family might be

initiated upon IL-7 stimulation in these cell lines, which might be a target for further explorations.

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3.2.5. Representative target of the p38 MAPK stress pathway: p38 MAPK

Withdrawal of IL-7 has been shown to induce a stress pathway activating p38 MAPK (Rajnavolgyi

et al., 2002). Activation of p38 MAPK leads to impeded cell proliferation and an alkalinization of the

pH in the cell (Khaled et al., 1999).

In this study, the cell lines were deprived for 24h of growth factor before re-stimulation with IL-2 or

IL-7. After these 24h, a possible phophorylation of p38 MAPK (Thr180/Tyr182) was observed in

2E8 cells. The band of the phosphorylated protein is in agreement with the molecular weight of p38

MAPK (43kDa); however, it is not in concordance with the possible band of the unphosphorylated

protein. Thus, it is unclear, whether p38 MAPK was phosphorylated or not in 2E8 cells. In contrast,

a phosphorylation of p38 MAPK can clearly be excluded in PB-1 and Kit 225 cells (see figure 56).

p38 MAPK p-p38 MAPK

kDa

98

64

50

36

kDa

250

9864

5036

16 16

Figure 56. Western blotting analysis of p38 MAPK and phospho-p38 MAPK in Kit 225, PB-1 and 2E8 cells. Cells were either incubated 10min at 37°C with 100ng/mL IL-7 or IL-2 or used untreated, followed by immunoblotting with anti-p38 MAPK and anti-phospho-p38 MAPK antibodyies as described under Materials and Methods. The figure shows that p38 MAPK phosphorylation (MW ≈ 43kDa) is only induced in 2E8 cells after 24h starvation time without growth factor. Unfortunately, no adequate pos. C. was found untreated Kit 225 cells served as a neg. C.); however the detected signals are in good agreement with the molecular weight of p38 MAPK. The blots were developed using IR fluorescence and are one selected representative of three independent experiments.

Probably, the starvation time was not long enough or, in contrast, even too long, in order to activate

p38 MAPK in those cell lines. Thus, again, possible differences between the different cell lines

were detected, which have already been observed for other targets. Differences between 2E8 and

Kit 225 cells might be due to the differences between B and T cells, whereas differences between

2E8 and PB-1 cells might be explained by the different maturation stages since PB-1 cells are of an

earlier stage of B cell maturation than 2E8 cells. Furthermore, 2E8 cells are IgM positive, whereas

PB-1 cells are not. The resulting differences in their biological responses have already been

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reported by Mire-Sluis et al. (2000). Moreover, the IL-7Rα density was higher on 2E8 cells in

comparison to the other cell lines, resulting probably in a stronger reaction of those cells.

Another indicator that p38 MAPK was really phosphorylated in 2E8 cells after 24h starvation time

was the fact that the signal decreased after re-addition of IL-7. Thus, the signal mainly disappeared

after 3h incubation time with IL-7 (see figure 57). It can be concluded, that p38 MAPK is induced

upon IL-7 withdrawal and specifically reduced upon IL-7 stimulation in this cell line.

Kit 225 stimulated with IL-2 and IL-7 2E8 and PB-1 stimulated with IL-7

kDa

250

98

6450

36

16

kDa

98

64

50

36

16

250

Figure 57. Kinetic measurements of p38 MAPK phosphorylation. Cells were incubated with IL-7 and IL-2 for the indicated time points between 10min and 6h. In 2E8 cells, the figure shows an IL-7 mediated down-regulation of phospho-p38 upon longer incubation times. The signal mainly disappeared after 3h incubation time. In the other cell lines no effect could be seen. The blots were developed using IR fluorescence and are one selected representative of two independent experiments.

Another cell line, in which p38 MAPK was induced upon IL-7 withdrawal was the D1 cell line

(Rajnavologyi et al., 2002). In these cells, phosphorylation of p38 MAPK was already induced after

4 - 6h (Khaled et al., 2001) and 2h (Rajnavologyi et al., 2002) of IL-7 withdrawal, respectively, and

resulted in expression of jun and fos family members and enhanced activator protein (AP)-1

activity, contributing to cell death.

Thus, the starvation time of 24h should in any case be long enough to activate p38 MAPK. It is

however possible, that this starvation time was even too long. In Kit 225 and PB-1 cells, it might

probably be of interest to study different starvation times without growth factor, in order to see

whether p38 MAPK could be induced upon longer or shorter time points.

3.3. Summary and Conclusions

The aim of this study was to select a target, which is suitable for development of a phosphorylation

assay and to shed light on the IL-7 signal transduction pathways due to the scarce literature reports

about this particular cytokine. Therefore, representative targets of some of the most important

pathways, presumed to be activated by IL-7, were selected and analyzed by using three different

cell lines.

Four investigated targets, STAT1, STAT3, AKT and ERK were activated upon IL-2 stimulation only,

not upon IL-7 stimulation, even if those two cytokines were presumed to initiate similar pathways,

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since both contain the common c chain and react in a comparable manner. However, there are

nevertheless differences between those two cytokines, already reported by others (e.g. Rosenthal

et al., 1997; Osborne et al., 2007) and confirmed in this study. This might probably inter alia be due

to the lacking -chain of the IL-7R.

Different expression pattern could be observed between the different cell lines since bcl-2, Lck and

Bim were expressed in the two B cell lines PB-1 and 2E8 only, and not in the T cell line Kit 225.

However none of these targets was specifically regulated by IL-7. The reason for this remains

unclear since some of the up-stream molecules such as STAT5 were activated by IL-7 and IL-2

stimulation. Furthermore, 2E8 is the only cell line, in which p38 MAPK was induced after 24h

starvation time and regulated by IL-7.

In this study, the only pathway identified to be induced in all three cell lines by IL-7, is the STAT5

pathway and the associated up-regulation of pim-1. STAT5 seems thus to be the most promising

target for development of a phosphorylation assay, especially due to the fast phosphorylation

reaction. A gene-expression assay using the up-regulation of pim-1 would of course equally be

possible but would take much more time (several hours in contrast to mapprox. 10min incubation

time with IL-7 for the STAT5 phosphorylation assay). In the STAT5/pim-1 pathway, only slight

differences in kinetics could be observed between the different cell lines. In Kit 225 cells, IL-7

induced phosphorylation was much weaker than IL-2 induced phosphorylation, which was in good

agreement with the IL-2R and IL-7R densities observed in the flow cytometric analyses. STAT5

phosphorylation could be inhibited by WP1066 in Kit 225 and 2E8 cells. In contrast, it was not

inhibited in PB-1 cells, showing another difference between the three cell lines.

Table 24 presents an overview, which of the analyzed targets of the IL-7 signaling pathways were

expressed in and activated (up-/down-regulated or phosphorylated) in the different cell lines

investigated.

Table 24. Summary of western blotting results.

Target Expressed in Activated in

Kit 225 PB-1 2E8 Kit 225

by IL-2

Kit 225

by IL-7

PB-1 by

IL-7

2E8 by

IL-7

STAT1 √ √ √ √ - - -

STAT3 √ √ √ √ - - -

STAT5 √ √ √ √ √ √ √

Pim-1 - - - √ √ √ √

Bcl-2 - √ √ - - - -

AKT √ √ √ √ - - -

Lck - √ √ - - - -

ERK √ √ √ √ - - -

Bim - √ √ - - - -

p38 MAPK √ √ √ - - - √

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It can be concluded, that this study serves as a systematic and thorough study of the most

important signaling pathways of IL-7 in the three cell lines that were investigated. Interesting

differences were observed between different cell lines and between the two c cytokines IL-2 and

IL-7. However, it remains to be clarified why some of the pathways, presumed to be activated by

IL-7, were not induced by IL-7 stimulation. STAT5 has been emphasized to be probably the most

important signaling pathway of IL-7 before (Goetz et al., 2004), and this study confirms this

hypothesis. STAT5 was consequently selected for development of an intracellular phosphorylation

assay, described in the following section.

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4. DEVELOPMENT OF A STAT5 PHOSPHORYLATION ASSAY AS AN ALTERNATIVE TO THE

CLASSICAL PROLIFERATION ASSAYS

Usually, the parameters used for determination of the biological activity are survival or proliferation

of the cell. However, the disadvantage of these classical “endpoint-assays” is that they require very

long incubation times, up to several days, since they measure the downstream events of a cellular

response. Additionally to the long incubation time, this might lead to a higher variability of the assay

(Sadick et al., 1999).

The colorimetric proliferation assay, which was developed previously for QC of Fc-IL7 at Merck

Serono, takes eight days until finalization. Moreover, it suffers from a poor robustness, since the

dynamic range (OD difference between the highest and the lowest value of the dose-response

curve) is not wide enough. As a consequence, many assays fail the set acceptance criteria

because of too low OD differences. Therefore, there is the need for a faster and more robust assay

format.

Using western blotting, STAT5 was identified as a target of IL-7 signaling in Kit 225 cells (see

section IV.3.) and a STAT5 phosphorylation assay was developed for this target. Detection of EPO-

induced phosphorylation of STAT5 in HEL/EpoR cells has for example already been used by the

SureFire™ assay (Perkin Elmer, Waltham, MA), utilizing the AlphaScreen® (Perkin Elmer)

technology or by a microsphere-based flow cytometry phospho-STAT5 assay using xMAP®

(Luminex® Corp., Austin, TX) technology in high-throughput screening (HTS) applications (Binder

et al., 2008).

The assay, which was developed in this study, is an ELISA based assay, using two different

microtiter-plates, one for cell stimulation and lysis, the other one for the ELISA. The procedure is

mainly based on the “Kinase receptor activation” (KIRA) assay, measuring ligand-induced receptor

tyrosine kinase activation in terms of receptor phosphorylation. This assay was developed by

Sadick et al. (1996, 1997, and 1999) as an alternative to endpoint-assays. It assesses the initial

events of the cellular response, which happen directly after the ligand binds to the receptor. The

KIRA assay is a highly reproducible and fast assay, showing a high correlation to the classical

proliferation assays (Sadick et al., 1999). In contrast to the KIRA assay, the STAT5

phosphorylation assay measures the intracellular signal transduction pathways, which are induced

directly after receptor activation. Moreover, it should also be suitable for use of suspension cells

since the original KIRA assay was developed for adherent cells only. The aim of this study was it

thus to develop a reliable, accurate and fast alternative to the classical proliferation assay for IL-7.

4.1. Assay development and optimization

The final assay was performed as described under Materials and Methods. A schematic diagram is

shown in figure 58.

During assay optimization, different parameters were varied. The experiments were run in

triplicates to confirm the results. A high OD difference between 100ng/mL IL-7 and the control

(0ng/mL IL-7) was used as a quality criterion in order to identify the best conditions.

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Coating of ELISA plate over

night with capture antibody

(100µL/well, 4°C)

Washing

90min

Blocking with 1% BSA

Washing

1

2

+

Stimulation of starved cells with IL-7

(10 - 15min, 37°C)

Addition of lysis buffer

60min

3

4

Transfer of cell lysate to ELISA

plate (85µL/well)

over night (4°C)

Addition of detection

antibody (100µL/well)

Washing

Incubation5

7

6

60min

Washing

Addition of secondary HRP-

conjugated antibody

(100µL/well)

60min

Addition of TMB

(100µL/well)

Stop reaction with

H2SO4 (100µL/well)

Washing

20min

Measurement of absorption

at 450nm

8

9

10

anti-p-STAT5 capture antibody

Cell lysate containing p-STAT5

anti-STAT5 detection antibody

secondary HRP-conjugated

anti-rabbit antibody

ELISA plate 96 well cell culture plate

Cell lysis

Kit 225 cells IL-7

Figure 58. Schematic diagram of the STAT5 phosphorylation assay. The assay was performed using two separate microtiter plates: the first one for cell stimulation and lysis, the second one for ELISA.

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During assay optimization, different compositions of the blocking buffer were tested using 0.5%,

1% and 2% BSA. However, the composition did not influence the results induced by 100 ng/mL IL-

7 since mean OD differences of 0.86 (0.5% BSA), 0.93 (1% BSA) and 0.90 (2% BSA) were

observed. Variation of the blocking time (30min steps between 1h and 3h) showed a maximum of

the mean OD difference after 90min incubation time by the 100ng/mL IL-7 positive control (see

figure 59). Thus, the blocking time was fixed to 90min using 1% BSA in DPBS.

Variation of blocking times

0

0,2

0,4

0,6

0,8

1

1,2

1,4

1,6

1,8

1h 1.5h 2h 2.5h 3h

blocking time

OD

valu

es

100ng/mL IL-7

Control

Figure 59. Variation of blocking times. The plate was incubated with blocking buffer (1% BSA in DPBS) for several times between 1h and 3h. The highest OD difference was reached after 1.5h. The shown data are mean values derived from three independent experiments; error bars indicate the mean standard deviations.

Moreover, different cell densities and starvation conditions for Kit 225 cells were tested.

Cell densities of 5x104 cells/well, 1x10

5 cells/well, 2x10

5 cells/well, 5x10

5 cells/well and 1x10

6

cells/well were stimulated with 100ng/mL IL-7 (see figure 60). Mean OD differences increased

strongly from 0.4 (5x104 cells/well) to 1.7 (5x10

5 cells/well) and then remained constant when

higher cell densities were used. The cell density was consequently fixed to 5x105 cells/well

resulting in a higher consumption of cells in comparison to the proliferation assay as the latter

assay needed only 1x105 cells/well.

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Variation of cell densities

0

0,5

1

1,5

2

2,5

3

5x104cells/well1x105cells/well2x105cells/well5x105cells/well1x106cells/well

cell density

OD

valu

es

100ng/mL IL-7

control

Figure 60. Variation of cell densities. The assay was performed using cell densities of 5x10

4, 1x10

5, 2x10

5, 5x10

5 and 1x10

6 cells/well. Mean OD

differences increased strongly from 0.4 (5x104

cells/well) to 1.7 (5x105 cells/well) and then remained constant

when using higher cell densities. The shown data are mean values derived from three independent experiments; error bars indicate the mean standard deviations.

Cells were starved three to four days in AIM-V Medium or one day only in RPMI 1640 medium

without growth factor. The RPMI medium was supplemented with 10% FBS or without FBS (see

figure 61).

Variation of starvation conditions

0,00

0,20

0,40

0,60

0,80

1,00

1,20

1,40

1 day in RPMI1640

with FBS (5x105

c/well)

1 day in RPMI1640

without FBS (5x105

c/well)

4 days in AIM-V (5x105

c/well)

starvation conditions

OD

valu

es

100ng/mL IL-7

control

Figure 61. Variation of starvation conditions Proir to the assay, cells were starved four days in AIM-V Medium or one day only in RPMI 1640 medium without growth factor. The RPMI medium was supplemented with 10% FBS or without FBS. The best starvation condition was one day in RPMI supplemented with 10% FBS. The shown data are mean values derived from three independent experiments; error bars indicate the mean standard deviations.

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Results after stimulation with 100ng/mL IL-7 indicated that the best starvation condition was one

day in RPMI supplemented with 10% FBS. A mean OD difference of 0.8 could be reached; in

contrast cells starved for both three days in AIM-V or for one day in RPMI 1640 without FBS

resulted in mean OD differences of only 0.5.

One possible reason for the lower OD difference of cells starved in RPMI without FBS in

comparison to the cells cultivated in medium supplemented with FBS might be the lower viability of

the cells which was only about 65 - 70% in contrast to at least 90% of the cells cultivated with FBS.

As a consequence, Kit 225 cells were starved 1 day without growth factor in RPMI 1640 + 10%

FBS in a density of 5x105 cells/mL.

Modifications were also necessary in order to generate crude lysates. Kit 225 cells are suspension

cells. In contrast to an assay using adherent cells, cells need to be collected by centrifugation first

and lysis of the cells has to take place in solution whereas for adherent cells, medium can be

removed by aspiraton and the lysis buffer can be added directly to the cell layer. Accordingly, some

modifications of the assay procedure were necessary such as direct addition of 20µL of 5 fold

concentrated lysis buffer (without centrifugation) to each well of the 96 well plate.

Furthermore, lysis time, incubation time with cell lysate and incubation time with detection antibody

were optimized.

Variation of the lysis time using incubation times of 15min, 30min, 60min and 90min, showed a

clear maximum in the OD difference after 60min stimulation with 100ng/mL IL-7 (see figure 62).

The OD difference increased up to 60min and decreased after longer incubation times. Thus, the

lysis time was fixed to 60min.

Variation of lysis times

0

0,2

0,4

0,6

0,8

1

1,2

1,4

15min 30min 60min 90min

incubation time

OD

valu

es

100ng/mL IL-7

Control

Figure 62. Variation of lysis times. The plate was incubated with 5 fold concentrated lysis buffer for 15min, 30min, 60min and 90min. The highest OD difference was reached after 60min. The shown data are mean values derived from three independent experiments; error bars indicate the mean standard deviations.

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The incubation time with cell lysate - from cells that had been stimulated with 100 ng/mL IL-7 or

used unstimulated - was varied using incubation times of 1h, 2h and 3h (see figure 63). Since the

highest OD difference could be reached after 1h incubation time (0.98 in contrast to 0.75 after 2h

and 0.65 after 3h), the incubation time was shortened from 2h to 1h.

Variation of incubation times with cell lysate

0,00

0,20

0,40

0,60

0,80

1,00

1,20

1,40

1,60

1,80

1h 2h 3h

incubation time

OD

valu

es

100ng/mL IL-7

Control

Figure 63. Variation of incubation times with cell lysate. The plate was incubated with cell lysate for 1h, 2h and 3h. The highest OD difference was reached after 1h. The shown data are mean values derived from three independent experiments; error bars indicate the mean standard deviations.

The plate was incubated with anti-STAT5 detection antibody over night at 4°C. Shorter incubation

times with detection antibody were equally tested in order to see whether it was possible to

complete the assay on the same day. This was feasible; however, it implicated lower OD

differences. After 2h and 5h incubation time at RT, OD differences of 0.5 and 0.6 were measured,

respectively; in contrast after incubation over night at 4°C, a mean OD difference of 0.9 could be

observed (see figure 64). It is thus more advantageous to incubate the plate with detection

antibody over night.

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Variation of incubation times with detection antibody

0

0,2

0,4

0,6

0,8

1

1,2

1,4

2h at RT 5h at RT over night (ca. 16-18h)

at 4°C

incubation time

OD

valu

es

100ng/mL IL-7

Control

Figure 64. Variation of incubation times with anti-STAT5 detection antibody. The plate was incubated with anti-STAT5 detection antibody for 2h (RT), 5h (RT) or over night (4°C). The highest OD difference was reached upon incubation over night. The shown data are mean values derived from three independent experiments; error bars indicate the mean standard deviations.

Another important step was the optimization of the secondary HRP conjugated antibody. The

choice of the secondary antibody had a major influence on the assay results: Thus OD differences

between 0.12 and 0.62 were obtained dependent on the source of the secondary HRP conjugated

antibody (see figure 65).

Variation of secondary HRP conjugated antibodies

0,00

0,20

0,40

0,60

0,80

1,00

1,20

sec. Ab from Kit (CellSignaling, 1:

1000)

sec. Ab (Promega, 1: 2500)

secondary antibody source

OD

valu

es

100ng/mL IL-7

control

Figure 65. Variation of secondary HRP conjugated antibodies. The assay was performed using a secondary antibody from two different sources. By replacing the antibody, an approx. 4-5 fold increase in the OD difference could be noticed. The shown data are mean values derived from three independent experiments; error bars indicate the mean standard deviations.

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131

Higher concentration of the chosen secondary antibody (1:1,000 instead of 1:2,500) did not lead to

a further increase of the OD difference since both, OD values of the sample and the control rose in

a similar way.

The incubation time with secondary HRP conjugated antibody was also varied (see figure 66). OD

differences increased from 30min (0.6) to 45min (0.8) and reached a plateau after 60min (1.1)

(75min: 1.0). Thus, the incubation time was set to 60min.

Variation of incubation times with secondary antibody

0

0,5

1

1,5

2

2,5

30min 45min 60min 75min

incubation time

OD

valu

es

100ng/mL IL-7

control

Figure 66. Variation of incubation times with secondary HRP conjugated antibody.

The plate was incubated with secondary HRP conjugated antibody for 30min, 45min, 60min and 75min. The highest OD difference was reached after 60min. The shown data are mean values derived from three independent experiments; error bars indicate the mean standard deviations.

Variation of the incubation time with TMB showed mean OD differences of 0.6 (5min), 0.8 (10min),

0.9 (15min), 1.0 (20min) and 1.0 (25min) (see figure 67). As a consequence, slightly longer

incubation times with TMB of about 20min seem to be more advantageous.

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Variation of incubation times with TMB

0

0,2

0,4

0,6

0,8

1

1,2

1,4

1,6

1,8

5min 10min 15min 20min 25min

incubation time

OD

valu

es

100ng/mL IL-7

control

Figure 67. Variation of incubation times with TMB.

The plate was incubated with TMB for various times between 5min and 25min. The highest OD difference was reached after 20min. The shown data are mean values derived from three independent experiments; error bars indicate the mean standard deviations.

At the end of assay optimization, the appropriate concentration range of Fc-IL7 was determined.

The concentration range was adapted to 0.4 – 100ng/mL; a representative curve is shown in figure

68.

0

0,5

1

1,5

2

2,5

0,1 1 10 100 1000

y

x

Standard Curve

Concentration [ng/mL]

OD

valu

es

at490nm

Figure 68. Concentration curve of the STAT5 phosphorylation assay.

The concentration range of the STAT5 phosphorylation assay was evaluated to be 0.4 – 100ng/mL cytokine fusion protein containing IL-7. The resulting, representative curve is shown in figure 68. Green points indicate the individual results, red points the mean values of the triplicates.

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4.2. Assay qualification

After assay development and optimization, the assay was qualified with respect to accuracy and

precision. For this purpose, three repetitions were performed on three different sample

concentrations of 50%, 100% and 150% in comparison to the 100% 100 ng/mL IL-7 standard (n =

9). The assays were performed independently on different days.

Qualification results showed a good recovery with a mean value of 101.9% and a low mean RE of

7.1%. The precision of the assay was with a mean CV of 8.9% high. An overall summary of the

qualification results is shown in table 25.

Table 25. Results of assay qualification.

Sample

concentration

Individual

potency

results

Mean Recovery

[%] RE [%] SD [%] CV [%]

50%

(rel.potency: 0.5)

(n = 3)

0.586

0.442

0.482

0.503 100.7 10.8 7.4 14.8

100%

(rel.potency: 1.0)

(n = 3)

0.998

1.066

1.028

1.031 103.1 3.2 3.4 3.3

150%

(rel. potency: 1,5)

(n = 3)

1.591

1.618

1.374

1.528 101.8 7.4 13.4 8.8

Overall summary

(n = 9) - 1.019 101.9 7.1 8.1 8.9

Results at the low and the high concentration level (50% and 150%) showed a bit larger deviations

from the expected concentration. Thus an RE of 10.8% and a CV of 14.8% were assessed for the

50% concentration level. For the 150% concentration level, an RE of 7.4% and a CV of 8.8% were

calculated. In contrast, results of the 100% concentration level were more accurate and precise,

showing a mean RE of 3.2% and a mean CV of 3.4%.

Nevertheless, REs and CVs for all concentration levels were all in the acceptable range of ± 30%,

which is usually applied for bioassays.

It can be concluded, that the STAT5 phosphorylation assay is a very accurate and precise assay,

being suitable for use in quality control. It can serve as alternative to the classical proliferation

assay.

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4.3. Comparison of the STAT5 phosphorylation assay to the proliferation assay

By comparing the STAT5 phosphorylation assay to the originally used colorimetric proliferation

assay, it was observed, that more cells were needed for the phosphorylation assay: 5x105

cells/well versus 1x105 cells/well for the proliferation assay. This is due to the lower sensitivity of

the phosphorylation assay in comparison to the end-point assay. Similar observations have already

been made for the KIRA assay. Sadick et al. (1999) estimated this assay to be about ten times less

sensitive than end-point assays. The higher sensitivity of the end-point assay was most likely

caused by the signal amplification provided by the kinase cascade. The lower sensitivity of the

STAT5 phosphorylation assay in comparison to the proliferation assay might be explained by the

same fact since the STAT5 phosphorylation is one of the first steps in the kinase cascade.

The higher number of cells needed for the phosphorylation assay leads to higher costs for the cell

culture. Moreover, the costs of the reagents needed for the phosphorylation assay, especially for

the antibodies, are much higher than for the colorimetric proliferation assay.

The advantage of the phosphorylation assay is that it is completed much faster than the

proliferation assay. The proliferation assay needs three days starvation of the cells in AIM-V

medium, one day to perform the assay plus four days incubation time with API. It takes thus eight

days to complete the assay. In contrast, for the phosphorylation assay, cells are seeded and

starved and the ELISA plate is coated on the first day, and the assay is performed on the second

day. It can either be finalized on the same day – implying however, lower OD differences, which

might lead to a lower precision and robustness of the assay – or be completed on the third day. It

can be concluded that – even if a reduction of the starvation time from three days to one day would

be equally possible for the proliferation assay – the assay procedure time is at least reduced from

six to three days by using the phosphorylation instead of the proliferation assay.

Another benefit of the phosphorylation assay is its higher robustness. The proliferation assay

showed sometimes very low OD differences below 0.5. As a consequence, many assays failed the

acceptance criteria, because the OD differences were too low. This is not the case for the

phosphorylation assay showing usually OD differences above 0.7, even up to 1.5. The problem of

the low robustness can thus be resolved by replacing the proliferation by the phosphorylation

assay.

4.4. Conclusions

As an alternative to classical proliferation assays, a rapid phosphorylation assay was developed,

measuring IL-7 induced STAT5 phosphorylation in Kit 225 cells. The assay is very accurate and

precise with a mean RE of 7.1% and a mean CV of 8.9%. Consequently, this assay serves as a

good and reliable alternative to classical end-point assays and is well-suited for use in QC of

biopharmaceuticals.

Despite of the higher costs of this assay - needed for cell culture and reagents - it has the

advantage to be much faster and more robust than the proliferation assay. The total time of the

assay could be reduced at least from six to three days. The OD differences obtained for the

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negative and positive control increased from values below 0.5 for the proliferation assay to values

above 0.7, and even up to 1.5, for the STAT5 phosphorylation assay. In addition, the signal to

noise ratios rose from values around 1.5 – 1.8 for the proliferation assay to values about 2.3 – 3.3

for the STAT5 phosphorylation assay. Signal to noise ratios above 2.0 are recommended for

bioassays.

The assay has been developed for a cytokine fusion protein containing IL-7 but could also be used

for other ligands inducing the JAK/STAT pathway and thus STAT5 phosphorylation, leading to a

more universal application of the assay. Moreover, it should be possible to further expand the

applicability of the assay by replacing STAT5 by another intracellular target, e.g. of the PI3K/AKT

or the Ras/Raf/ERK pathway. As a consequence, the assay format could be used for many

different classes of biopharmaceuticals.

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136

VV.. OOVVEERRAALLLL CCOONNCCLLUUSSIIOONNSS AANNDD OOUUTTLLOOOOKK

Biopharmaceuticals such as antibodies or cytokine fusion proteins are of growing interest in anti-

cancer therapy. In order to ensure consumer and patient safety, the quality of these products

needs to be controlled according to national and international guidelines. The major factors under

which the product is characterized are its purity, stability, safety and potency. The method of choice

for QC of biological products with regards to their potency is the use of biological assays, making

them to a very important instrument in pharmaceutical industry without which the development of

novel pharmaceuticals would not be possible.

The aim of this study was to optimize existing methods for biological assays and to implement

alternative assay formats. The methods were characterized according their sensitivity, accuracy,

precision, linearity and reproducibility.

First of all, analysis methods and read-out systems for proliferation assays, usually applied for QC

of biopharmaceuticals, were compared. The aim was it to find the best analysis model and the

most appropriate read-out system beyond the methods investigated.

Regarding the comparison of the analysis models, the parallel line model, which was used for QC

purposes at Merck Serono before, was opposed to the logistic models, four- and five parameter fit.

The results of this comparison revealed a slightly better accuracy and precision of the logistic

models in comparison to the PL model; however, differences were not significant. On the other

side, the logistic models showed a significantly higher failure rate, including all assays with failed

tests of linearity or parallelism according to preset acceptance criteria. As a consequence, no clear

recommendation for the appropriate analysis model can be given. All of the three models are suited

well for analysis of potency assays. The choice of the model has to be made individually and

depends on the performed type of assay set up. It can not be concluded, which of the models will

be the most commonly applied model in future. Besides, it has to be remembered that there are

other models like the slope ratio assay or comparison of EC50 values, which might equally be used

instead of the models tested in this study, even if the PL, 4PL and 5PL models are the mainly used

calculation models to date.

Regarding the comparison of read-out systems, it was tested in this study, whether luminescence

or fluorescence systems could be of advantage in comparison to the colorimetric system, originally

in use for detection of proliferation assays at Merck Serono. According to the results of this study,

both, the luminescence and fluorescence system, that is CellTiter- Glo®

and Alamar BlueTM

, were

much more sensitive in comparison to the colorimetric MTS/PMS assay. The signal to noise ratios,

which are a surrogate parameter for the robustness of an assay, were the lowest for the

colorimetric system and the highest for the luminescence technique. In comparison to the Alamar

Blue assay, which needs several hours to be completed, the ATP assay has the advantage to be

much faster since the plate can already be measured 5 - 10min after addition of substrate. These

factors make the luminescence read-out the most promising of the three methods investigated,

even if all three methods are suited well for use in QC, since they produce reliable and reproducible

results. The detriment of the little higher costs of the CellTiter- Glo®

reagent in comparison to the

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137

MTS/PMS reagent should easily be balanced by the higher sensitivity, robustness and rapidness of

this assay. As a consequence, it would be of advantage to use the luminescence read-out for

development of future assays and to probably even replace the MTS/PMS reagent by CellTiter-

Glo® for assays already in place.

As an alternative to the commonly used proliferation assays, an intracellular phosphorylation assay

was developed for Fc-IL7, since the originally used proliferation assay suffered from a very long

incubation time and a poor robustness. In order to find a target for development of the

phosphorylation assay, the IL-7 signaling pathways were screened by western blotting. A

thourough study was done since relatively little was known about this cytokine, making it to an

interesting target for further explorations. Consequently, the IL-7 signaling pathways were

compared in three different cell lines (PB-1, 2E8 and Kit 225). In addition, the IL-7 pathways were

opposed to the IL-2 pathways. The results of the study revealed interesting differences between

the different cell lines, especially in the expression pattern of several proteins. Regarding the

comparison of the two γc cytokines, some pathways were initiated by IL-2 only, and not by IL-7.

The only pathway identified in this study to be induced in all three cell lines by IL-7, was the STAT5

pathway and the associated induction of pim-1. STAT5 has been emphasized to be probably the

most important signaling molecule of IL-7 before (Goetz et al., 2004), and this study confirms this

hypothesis. Nevertheless, other signaling pathways need to be involved in IL-7 signaling, especially

because the activation of STAT5 is supposed not to induce proliferation of cells (Isaksen et al.,

2002). But which other pathways are these? At least in this study and in the three cell lines

investigated, no other pathway could be identified. The IL-7 signaling pathways are thus not

completely elucidated and are worth to be studied further.

According to the western blotting analyses, STAT5 was identified as the most appropriate target for

development of a phosphorylation assay. The developed STAT5 phosphorylation assay was very

accurate and precise. It can serve as a good and reliable alternative to classical end-point assays

and is well-suited for use in QC of biopharmaceuticals. The main advantage of this assay are its

rapidness - reducing the total time of the assay from six to three days – and the higher robustness

in comparison to the proliferation assay. The applicability of the assay might be expanded by

replacing STAT5 by other intracellular targets making the assay format suitable for QC of many

different classes of biopharmaceuticals. The development of such assays might be of interest for

new projects. However, the costs of the phosphorylation assay are much higher in comparison to

the proliferation assay, making it difficult to implement those assays for routine use. Nevertheless,

the STAT5 phosphorylation assay is an interesting alternative assay format. In addition to the

phosphorylation assays, other innovative assay formats like reporter gene assays might be

interesting to be developed and to be compared to the assays already in place in order to

implement new technologies and to benefit of the possible advantages.

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LIST OF FIGURES

Figure 1. 3D structure of the IL-7 receptor. ................................................................................. 22

Figure 2. Illustration of the most important IL-7 signaling pathways. ...................................... 24

Figure 3. Overview of assay formats. ........................................................................................... 35

Figure 4. Graphical presentation of the parallel line model. ...................................................... 36

Figure 5. Graphical presentation of the four-parameter fit. ....................................................... 37

Figure 6. Reaction equation of the colorimetric read-out. ......................................................... 39

Figure 7. Reaction equation of the fluorescence read-out. ....................................................... 40

Figure 8. Reaction equation of the luminescence read-out. ...................................................... 40

Figure 9. Microscopic images of the cell lines, used in this study. .......................................... 43

Figure 10. General plate layout for potency assays. .................................................................. 52

Figure 11. Concentration ranges of the CTLL-2 potency assay. ............................................... 59

Figure 12. Plot of the pooled standard deviations (n = 18) vs. the measured mean responses

for each concentration point. ........................................................................................................ 61

Figure 13. Plot of the pooled standard deviations (n = 18) vs. the dose squared for each

concentration point. ....................................................................................................................... 62

Figure 14. Individual, representative graphs (calculated by PLA) of a CTLL-2 potency assay.

.......................................................................................................................................................... 63

Figure 15. Results CTLL-2 potency assay: expected activity 50%. .......................................... 64

Figure 16. Results CTLL-2 potency assay: expected activity 100%. ........................................ 65

Figure 17. Results CTLL-2 potency assay: expected activity 150%. ........................................ 66

Figure 18. Concentration ranges of the DiFi potency assay. .................................................... 70

Figure 19. Plot of the pooled standard deviations (n = 18) vs. the measured mean responses

for each concentration point. ........................................................................................................ 71

Figure 20. Plot of the pooled standard deviations (n = 18) vs. the dose squared for each

concentration point. ....................................................................................................................... 72

Figure 21. Individual, representative graphs (calculated by PLA) of a DiFi potency assay. .. 73

Figure 22. Results DiFi potency assay: expected activity 50%. ................................................ 74

Figure 23. Results DiFi potency assay: expected activity 100%. .............................................. 75

Figure 24. Results DiFi potency assay: expected activity 150%. .............................................. 76

Figure 25. % REs [residuals/ measured response*100] of the 4PL and 5PL models for each

concentration point. ....................................................................................................................... 81

Figure 26. Illustration of the signal to noise ratio of a representative dose response curve. 85

Figure 27. Concentration curve of a CTLL-2 potency assay, detected by colorimetric read-

out. ................................................................................................................................................... 86

Figure 28. Optimized curve of a CTLL-2 potency assay, detected by colorimetric read-out. 86

Figure 29. Concentration curve of a CTLL-2 potency assay, detected by luminescence read-

out. ................................................................................................................................................... 87

Figure 30. Optimized curve of a CTLL-2 potency assay, detected by luminescence read-out.

.......................................................................................................................................................... 87

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Figure 31. Optimized curve of a CTLL-2 potency assay, detected by fluorescence read-out.

.......................................................................................................................................................... 88

Figure 32. Concentration curve of a DiFi potency assay, detected by colorimetric read-out.91

Figure 33. Concentration curve of a DiFi potency assay, detected by luminescence read-out.

.......................................................................................................................................................... 91

Figure 34. Concentration curve of a DiFi potency assay, detected by luminescence read-out.

.......................................................................................................................................................... 92

Figure 35. Concentration curve of a Kit 225 potency assay, detected by colorimetric read-

out. ................................................................................................................................................... 95

Figure 36. Optimized curve of a Kit 225 potency assay, detected by colorimetric read-out. . 95

Figure 37. Concentration curve of a Kit 225 potency assay, detected by luminescence read-

out. ................................................................................................................................................... 96

Figure 38. Optimized curve of a Kit 225 potency assay, detected by luminescence read-out.

.......................................................................................................................................................... 96

Figure 39. Flow cytometric analysis of IL-7Rα densities on A) Kit 225, B) PB-1, and C) 2E8

cells. ............................................................................................................................................... 103

Figure 40. Flow cytometric analysis of IL-2Rα densities on A) Kit 225, B) PB-1, and C) 2E8

cells. ............................................................................................................................................... 104

Figure 41. Flow cytometric analysis of IL-2Rβ densities on A) Kit 225, B) PB-1, and C) 2E8

cells. ............................................................................................................................................... 105

Figure 42. Western blotting analysis of STAT1 and phospho (p)-STAT1 in Kit 225, PB-1 and

2E8 cells. ....................................................................................................................................... 106

Figure 43. Western blotting analysis of STAT3 and phospho-STAT3 in Kit 225, PB-1 and 2E8

cells. ............................................................................................................................................... 107

Figure 44. Western blotting analysis of STAT5 and phospho-STAT5 in Kit 225, PB-1 and 2E8

cells. ............................................................................................................................................... 108

Figure 45. Kinetic measurements of STAT5 phosphorylation. ................................................ 109

Figure 46. Inhibition of STAT5 phosphorylation by WP1066. .................................................. 110

Figure 47. Western blotting analysis of pim-1 in Kit 225, PB-1 and 2E8 cells. ...................... 111

Figure 48. Kinetic measurements of pim-1 up-regulation. ....................................................... 112

Figure 49. Western blotting analysis of bcl-2 in Kit 225, PB-1 and 2E8 cells. ....................... 113

Figure 50. Western blotting analysis of AKT and phosphor-AKT in Kit 225, PB-1 and 2E8

cells. ............................................................................................................................................... 114

Figure 51. Kinetic measurements of AKT phosphorylation. .................................................... 115

Figure 52. Western blotting analysis of ERK and phospho-ERK in Kit 225, PB-1 and 2E8

cells. ............................................................................................................................................... 116

Figure 53. Kinetic measurements of ERK phosphorylation. ................................................... 116

Figure 54. Western blotting analysis of Bim and phospho-Bim in Kit 225, PB-1 and 2E8 cells.

........................................................................................................................................................ 118

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Figure 55. Western blotting analysis of Lck and phospho-Lck in Kit 225, PB-1 and 2E8 cells.

........................................................................................................................................................ 119

Figure 56. Western blotting analysis of p38 MAPK and phospho-p38 MAPK in Kit 225, PB-1

and 2E8 cells. ................................................................................................................................ 120

Figure 57. Kinetic measurements of p38 MAPK phosphorylation. ......................................... 121

Figure 58. Schematic diagram of the STAT5 phosphorylation assay..................................... 125

Figure 59. Variation of blocking times. ...................................................................................... 126

Figure 60. Variation of cell densities. ......................................................................................... 127

Figure 61. Variation of starvation conditions ............................................................................ 127

Figure 62. Variation of lysis times. ............................................................................................. 128

Figure 63. Variation of incubation times with cell lysate. ........................................................ 129

Figure 64. Variation of incubation times with anti-STAT5 detection antibody. ..................... 130

Figure 65. Variation of secondary HRP conjugated antibodies. ............................................. 130

Figure 66. Variation of incubation times with secondary HRP conjugated antibody. .......... 131

Figure 67. Variation of incubation times with TMB. .................................................................. 132

Figure 68. Concentration curve of the STAT5 phosphorylation assay. ................................. 132

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LIST OF TABLES

Table 1. Survey of cytokine families. ........................................................................................... 19

Table 2. Features of cytokines. ..................................................................................................... 20

Table 3. Results CTLL-2 potency assay: expected activity 50% (i.e. relative potency: 0.5). .. 64

Table 4. Results CTLL-2 potency assay: expected activity 100% (i.e. relative potency: 1.0). 65

Table 5. Results CTLL-2 potency assay: expected activity 150% (i.e. relative potency: 1.5). 66

Table 6. Summary of CTLL-2 assay results. ................................................................................ 68

Table 7. Results DiFi potency assay: expected activity 50% (i.e. relative potency: 0.5). ....... 74

Table 8. Results DiFi potency assay: expected activity 100% (i.e. relative potency: 1.0). ..... 75

Table 9. Results DiFi potency assay: expected activity 150% (i.e. relative potency: 1.5). ..... 76

Table 10. Summary of DiFi assay results. ................................................................................... 78

Table 11. Summary and comparison between the different models......................................... 83

Table 12. Results qualification CTLL-2 assay: expected activity 50% (i.e. relative potency:

0.5). .................................................................................................................................................. 89

Table 13. Results qualification CTLL-2 assay: expected activity 100% (i.e. relative potency:

1.0). .................................................................................................................................................. 89

Table 14. Results qualification CTLL-2 assay: expected activity 150% (i.e. relative potency:

1.5). .................................................................................................................................................. 89

Table 15. Summary of CTLL-2 assay parameters and comparison between the different read-

out systems. .................................................................................................................................... 90

Table 16. Results qualification DiFi assay: expected activity 50% (i.e. relative potency: 0.5).

.......................................................................................................................................................... 93

Table 17. Results qualification DiFi assay: expected activity 100% (i.e. relative potency: 1.0).

.......................................................................................................................................................... 93

Table 18. Results qualification DiFi assay: expected activity 150% (i.e. relative potency: 1.5).

.......................................................................................................................................................... 93

Table 19. Summary of DiFi assay parameters and comparison between the different read-out

systems. .......................................................................................................................................... 94

Table 20. Results qualification Kit 225 assay: expected activity 50% (i.e. relative potency:

0.5). .................................................................................................................................................. 97

Table 21. Results qualification Kit 225 assay: expected activity 100% (i.e. relative potency:

1.0). .................................................................................................................................................. 97

Table 22. Results qualification Kit 225 assay: expected activity 150% (i.e. relative potency:

1.5). .................................................................................................................................................. 98

Table 23. Summary of Kit 225 assay parameters and comparison between the different read-

out systems. .................................................................................................................................... 99

Table 24. Summary of western blotting results. ....................................................................... 122

Table 25. Results of assay qualification. ................................................................................... 133

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APPENDIX:

STATISTICAL ANALYSIS OF BIOASSAY RESULTS: A COMPARISON BETWEEN DIFFERENT

CALCULATION MODELS

Author: Enrico Tucci

Researcher

National Institute of Statistics

Viale Liegi, 13 - 00198 Rome, Italy

Email: [email protected]

Tel.: +39 06 8522 7342

Cell.: +39 328 7518313

Statistical consultant

M&D - Management and Development srl

Via Andrea Del Castagno, 60 - 00142 Roma, Italy

Email: [email protected]

Tel +39 06 5911461

Fax: +39 06 5910274

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1. Objective

The aim of this report is to analyze the impact on the performance of the bioassay results obtained

in the department Analytical Development Biotech Products at Merck Serono in Darmstadt at:

different calculation Models

different Concentration levels

different Ranges.

Furthermore, this document verifies whether the difference obtained in the failure rates using

different calculation models is significant or not.

2. Definitions

Dependent variable: the observed variable in an experiment or study whose changes are

determined by the presence or degree of one or more independent variables.

Independent variable: the manipulated variable in an experiment or study whose presence or

degree determines the change in the dependent variable.

Stratification variable: the factor that can be used to separate data into subgroups in order to

analyse them separately and have separate results.

Results of Analyses: the dependent variable whose determinations are the bioassay results.

Concentration: the independent variable whose determinations are “0.5”, “1.0” and “1.5”.

Recovery: the dependent variable obtained by the ratio between the Results of Analyses and

the Concentration level.

Results of AnalysesRecovery =

Concentration Equation 1

Assay: the stratification variable whose determinations are “1” and “2”

Model: the independent variable whose determinations are “PL”, “4PL” and “5PL”.

Range: the independent variable whose determinations are “5-30ng/mL”, “0.75-100ng/mL”,

“6.8-80ng/mL” for the CTLL-2 potency assay and “2-12nM”, “0.25-95nM”, “5-55nM” for The DiFi

potency assay.

Plate: the stratification variable whose determinations are “1”, “2”, “3”, “4”, “5” and “6”.

3. Statistical Method

Since data refer to different concentration levels (0.5, 1.0 and 1.5), the statistical evaluation will be

performed using the recovery instead of the simple bioassay result.

In order to analyze the differences between the bioassay results at different levels of the

independent variables (calculation model, concentration level and range), an ANalysis Of VAriance

(ANOVA) has been performed. The aim of the ANOVA is, in fact, to test whether the averages of

the bioassay results obtained at different determinations of the independent variable are

statistically different or not. In other words, the One-Way ANOVA procedure is designed to

construct a statistical model describing the impact of a single categorical factor (for example,

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Model) on a dependent variable (Recovery). Tests are run to determine whether or not there are

significant differences between the means.

In the Anova:

Residuals are assumed to be normally distributed

Variance is assumed approximately constant for all factor levels.

Moderate departures from normality of the residuals are of little concern. It is useful to check the

residuals, though, because they are an opportunity to learn more about the data. In order to check

if the residuals can be adequately modelled by a normal distribution the Kolmogorov-Smirnov Test

has been used.

Variance Check is used in the One-Way ANOVA procedures to test the hypothesis that the

standard deviations within each group are equal. If the observations can be modelled by a normal

distribution, the Cochran‟s Test is more reliable. Otherwise the Levene‟s Test will be used.

Cochran‟s Test: compares the maximum within-sample variance to the average within-sample

variance. The test is appropriate only if all group sizes are equal.

Levene‟s Test: performs a one-way analysis of variance on the absolute differences between each

observation and its corresponding group mean.

A P-value<0.05 indicates a significant difference between the standard deviations.

4. Statistical evaluation

4.1. Results of the analyses by Model

4.1.1. CTLL-2 potency assay

The aim of this section is to analyze if the results obtained with different Model (PL 4PL, and 5PL)

are significant different or in other words, to determine whether or not the Model (PL, 4PL and 5PL)

has an impact on the Recovery for the CTLL-2 potency assay.

The ANOVA is used to analyze the relationships between different Models (PL 4PL, and 5PL) and

the Recovery obtained.

The Kolmogorov-Smirnov Test is a goodness of fit tests for residual. It determines whether residual

can be adequately modelled by a normal distribution.

Kolmogorov-Smirnov Test

Normal

DPLUS 0.12526

DMINUS 0.0563622

DN 0.12526

P-Value 0.0741446

Since the smallest P-value amongst the tests performed is greater than 0.05, we can not reject the

idea that Residual comes from a normal distribution with 95% confidence.

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Histogram for residuals

-0,33 -0,13 0,07 0,27 0,47

Residual

0

10

20

30

40fr

eq

ue

ncy

Distribution

Normal

The statistic displayed in this table tests the null hypothesis that the standard deviations of

Recovery within each of the 3 levels of Model (PL 4PL, and 5PL) is the same. Of particular interest

is the P-value. Since the P-value is greater than 0.05, there is not a statistically significant

difference amongst the standard deviations at the 95.0% confidence level.

Variance Check

Test P-Value

Cochran's C 0.476798 0.0538804

The ANOVA table decomposes the variance of Recovery into two components: a between-group

component and a within-group component. The F-ratio, which in this case equals 0.18815, is a

ratio of the between-group estimate to the within-group estimate. Since the P-value of the F-test is

greater than 0.05, there is not a statistically significant difference between the mean Recovery from

one level of Model to another at the 95.0% confidence level.

ANOVA Table for Recovery by Model

Source Sum of

Squares

Df Mean Square F-Ratio P-Value

Between groups 0.00747792 2 0.00373896 0.19 0.8288

Within groups 2.02697 102 0.0198722

Total (Corr.) 2.03445 104

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160

4PL 5PL PL

Means and 95,0 Percent Confidence Intervals (internal s)

Model

0,97

0,99

1,01

1,03

1,05

1,07

1,09

Re

co

ve

ry

This table shows the mean Recovery for each level of Model. It also shows the standard error of

each mean, which is a measure of its sampling variability. The standard error is formed by dividing

the standard deviation at each level by the square root of the number of observations at that level.

The table also displays an interval around each mean. The intervals currently displayed are 95.0%

confidence intervals for each mean separately. 95.0% of such intervals will contain the true means.

Table of Means for Recovery by Model with 95.0 percent confidence intervals

Stnd. error

Model Count Mean (individual) Lower limit Upper limit

4PL 26 1.02412 0.023186 0.976363 1.07187

5PL 25 1.02284 0.02355 0.974235 1.07144

PL 54 1.04035 0.0216765 0.996874 1.08383

Total 105 1.03216

4PL 5PL PL

Residual Plot for Recovery

-0,44

-0,24

-0,04

0,16

0,36

0,56

res

idu

al

Model

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The same calculations have also been made for each individual plate (plate 1-6) in order to see

whether significant differences between the different models could be observed when regarding

one individual assay result. These calculations are not shown in detail here, but are summarized in

the summary table for the CTLL-2 potency assay.

4.1.2. DiFi potency assay

The aim of this section is to analyze if the results obtained with Model (PL, 4PL and 5PL) are

significant different or in other words, to determine whether or not the Model (PL, 4PL and 5PL) has

an impact on the Recovery for the DiFi potency assay.

An ANalysis Of VAriance (Anova) is used to analyze the relationships between different Models

(PL, 4PL and 5PL) and the Recovery obtained. It compares the three models in order to see if any

of the model means is statistically different from the others in the DiFi potency assay.

The Kolmogorov-Smirnov Test is a goodness of fit tests for residual. It determines whether residual

can be adequately modelled by a normal distribution.

Kolmogorov-Smirnov Test

Normal

DPLUS 0.135552

DMINUS 0.0583647

DN 0.135552

P-Value 0.0292179

Since the smallest P-value amongst the tests performed is less than 0.05, we can reject the idea

that Residual comes from a normal distribution with 95% confidence.

Histogram for Residual

-0,26 -0,06 0,14 0,34 0,54

Residual

0

10

20

30

40

50

fre

qu

en

cy

Distribution

Normal

The statistic displayed in this table tests the null hypothesis that the standard deviations of

Recovery within each of the 3 levels of Model (PL, 4PL and 5PL) is the same. Of particular interest

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is the P-value. Since the P-value is greater than 0.05, there is not a statistically significant

difference amongst the standard deviations at the 95.0% confidence level.

Variance Check

Test P-Value

Levene's 2.09923 0.127347

The ANOVA table decomposes the variance of Recovery into two components: a between-group

component and a within-group component. The F-ratio, which in this case equals 0.378565, is a

ratio of the between-group estimate to the within-group estimate. Since the P-value of the F-test is

greater than 0.05, there is not a statistically significant difference between the mean Recovery from

one level of Model to another at the 95.0% confidence level.

ANOVA Table for Recovery by Model

Source Sum of

Squares

Df Mean Square F-

Ratio

P-Value

Between groups 0.0118103 2 0.00590517 0.38 0.6857

Within groups 1.74707 112 0.0155988

Total (Corr.) 1.75888 114

4PL 5PL PL

Means and 95,0 Percent Confidence Intervals (internal s)

Model

0,93

0,95

0,97

0,99

1,01

1,03

Re

co

ve

ry

This table shows the mean Recovery for each level of Model. It also shows the standard error of

each mean, which is a measure of its sampling variability. The standard error is formed by dividing

the standard deviation at each level by the square root of the number of observations at that level.

The table also displays an interval around each mean. The intervals currently displayed are 95.0%

confidence intervals for each mean separately. 95.0% of such intervals will contain the true means.

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Table of Means for Recovery by Model with 95.0 percent confidence intervals

Stnd. error

Model Count Mean (individual) Lower limit Upper limit

4PL 31 0.993871 0.0173448 0.958448 1.02929

5PL 30 0.991433 0.0182236 0.954162 1.0287

PL 54 0.972444 0.020291 0.931746 1.01314

Total 115 0.983174

4PL 5PL PL

Residual Plot for Recovery

-0,6

-0,4

-0,2

0

0,2

0,4

0,6

res

idu

al

Model

Comparable to the CTLL-2 potency assay, the same calculations have also been made for each

individual plate (plate 1-6) in order to see whether significant differences between the different

models could be observed when regarding one individual assay result. These calculations are not

shown in detail here, but are summarized in the summary table for the DiFi potency assay.

4.1.3. Conclusions

The ANOVA always shows that there is not a significant statistically difference between the means

from one level of Model to another at the 95.0% confidence level, except for the results of the Plate

2 (CTLL-2 potency assay).

As for the Plate 2 (CTLL-2 potency assay), the Variance Check shows that there is a statistically

significant difference amongst the standard deviations at the 95.0% confidence level. This violates

one of the important assumptions underlying the analysis of variance and invalidates the statistical

tests. Therefore the ANOVA can not be performed. In this case, the presence of 1 outside point

suggests using a more robust test which compares medians instead of means (Kruskal-Wallis

Test) and the result is that there is not a statistically significant difference amongst the medians at

the 95.0% confidence level.

Page 164: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

164

Summary Table for Model (CTLL-2 potency assay)

Comments

YES NO

Assay 1

Test for normality KS Test P-Value=0.07. The observation can be adequately

modeled by a normal distribution

Variance Check Cochran's P-Value=0.05.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.83. There is not a statistically

significant difference between the means

Assay 1 and Plate 1

Test for normality KS Test P-Value=0.44. The observation can be adequately

modeled by a normal distribution

Variance Check Cochran's P-Value=1.0.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.94. There is not a statistically

significant difference between the means

Assay 1 and Plate 2

Test for normality KS Test P-Value=0.56. The observation can be adequately

modeled by a normal distribution

Variance CheckCochran's and Bartlett's P-Value < 0.05.There is a

statistically significant difference amongst the standard

deviations

Test on Medians : Kruskal-

Wallis Test Kruskal-Wallis Test P-Value=1.0. There is not a statistically

significant difference amongst the medians

Assay 1 and Plate 3

Test for normality KS Test P-Value=0.75. The observation can be adequately

modeled by a normal distribution

Variance Check Cochran's P-Value=0.63.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.88. There is not a statistically

significant difference between the means

Assay 1 and Plate 4

Test for normality KS Test P-Value=0.95. The observation can be adequately

modeled by a normal distribution

Variance Check Cochran's P-Value=0.24.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.73. There is not a statistically

significant difference between the means

Assay 1 and Plate 5

Test for normality KS Test P-Value=0.80. The observation can be adequately

modeled by a normal distribution

Variance Check Cochran's P-Value=0.70.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.97. There is not a statistically

significant difference between the means

Assay 1 and Plate 6

Test for normality KS Test P-Value=0.54. The observation can be adequately

modeled by a normal distribution

Variance Check Cochran's P-Value=0.25.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.76. There is not a statistically

significant difference between the means

P-value > 0.05

Results of the analyses by Model

Page 165: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

165

Summary Table for Model (DiFi potency assay)

Comments

YES NO

Assay 2

Test for normality KS Test P-Value=0.02. The observation can't be adequately

modeled by a normal distribution

Variance Check Levene's P-Value=0.13.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.68. There is not a statistically

significant difference between the means

Assay 2 and Plate 1

Test for normality KS Test P-Value=0.35. The observation can be adequately

modeled by a normal distribution

Variance Check Cochran's P-Value=1.0.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.62. There is not a statistically

significant difference between the means

Assay 2 and Plate 2

Test for normality KS Test P-Value=0.91. The observation can be adequately

modeled by a normal distribution

Variance Check Cochran's P-Value=0.15.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.47. There is not a statistically

significant difference between the means

Assay 1 and Plate 3

Test for normality KS Test P-Value=0.51. The observation can be adequately

modeled by a normal distribution

Variance Check Cochran's P-Value=0.58.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.78. There is not a statistically

significant difference between the means

Assay 2 and Plate 4

Test for normality KS Test P-Value=0.60. The observation can be adequately

modeled by a normal distribution

Variance Check Cochran's P-Value=1.0.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.40. There is not a statistically

significant difference between the means

Assay 2 and Plate 5

Test for normality KS Test P-Value=0.28. The observation can be adequately

modeled by a normal distribution

Variance Check Cochran's P-Value=0.16.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.97. There is not a statistically

significant difference between the means

Assay 2 and Plate 6

Test for normality KS Test P-Value=0.65. The observation can be adequately

modeled by a normal distribution

Variance Check Bartlett's P-Value=0.09.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.31. There is not a statistically

significant difference between the meansKS=Kolmogorov-Smirnov

P-value > 0.05

Results of the analyses by Model

Page 166: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

166

4.2. Results of the analyses by Concentration

4.2.1. CTLL-2 potency assay

The aim of this section is to analyze if the results obtained with Concentration (0.5, 1.0 and 1.5) are

significant different or in other words, to determine whether or not the Concentration (0.5, 1.0 and

1.5) has an impact on the Recovery for the CTLL-2 potency assay.

An ANalysis Of VAriance (Anova) is used to analyze the relationships between different

Concentration (0.5, 1.0 and 1.5) and the Recovery obtained. It compares the three Concentrations

in order to see if any of the concentration means is statistically different from the others in the

CTLL-2 potency assay.

The Kolmogorov-Smirnov Test is a goodness of fit tests for residual. It determines whether

Residual can be adequately modelled by a normal distribution.

Kolmogorov-Smirnov Test

Normal

DPLUS 0.107995

DMINUS 0.0422386

DN 0.107995

P-Value 0.17278

Since the smallest P-value amongst the tests performed is greater than 0.05, we can not reject the

idea that Residual comes from a normal distribution with 95% confidence.

Histogram for Residual

-0,29 -0,09 0,11 0,31 0,51

Residual

0

10

20

30

40

fre

qu

en

cy

Distribution

Normal

The statistic displayed in this table tests the null hypothesis that the standard deviations of

Recovery within each of the 3 levels of Concentration is the same. Of particular interest is the P-

value. Since the P-value is less than 0.05, there is a statistically significant difference amongst the

standard deviations at the 95.0% confidence level. This violates one of the important assumptions

underlying the analysis of variance and will invalidate the statistical tests.

Page 167: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

167

Variance Check

Test P-Value

Cochran's C 0.518319 0.010969

Bartlett's 1.14048 0.00133671

This table shows the mean Recovery for each level of Concentration. It also shows the standard

error of each mean, which is a measure of its sampling variability. The standard error is formed by

dividing the standard deviation at each level by the square root of the number of observations at

that level. The table also displays an interval around each mean. The intervals currently displayed

are 95.0% confidence intervals for each mean separately. 95.0% of such intervals will contain the

true means.

Table of Means for Recovery by Concentration with 95.0 percent confidence intervals

Stnd. error

Concentration Count Mean (individual) Lower limit Upper limit

0.5 35 1.08217 0.0288667 1.02351 1.14084

1 36 1.01075 0.0149833 0.980332 1.04117

1.5 34 1.00335 0.0236528 0.955231 1.05147

Total 105 1.03216

0,5

1

1,5

Box-and-Whisker Plot

0,75 0,95 1,15 1,35 1,55

Recovery

Co

nce

ntr

ati

on

This graph shows 3 box-and-whisker plots, one for each level of Concentration. The rectangular

part of the plot extends from the lower quartile to the upper quartile covering the center half of each

sample. The center lines within each box show the location of the sample medians. The plus signs

indicate the location of the sample means. The whiskers extend from the box to the minimum and

maximum values in each sample except for any outside or far outside points, which will be plotted

separately. Outside points are points which lie more than 1.5 times the interquartile range above or

below the box and are shown as small squares. Far outside points are points which lie more than

Page 168: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

168

3.0 times the interquartile range above or below the box and are shown as small squares with plus

signs through them. In this case, there are 8 outside points. This might suggest the presence of

outliers.

Therefore, it is strongly recommended when the result of a test is so sensitive to outliers the use of

the less sensitive test. In this case a test on the medians has been chosen (Kruskal-Wallis Test)

which compares medians instead of means.

Kruskal-Wallis Test for Recovery by Concentration

Concentration Sample Size Average Rank

0.5 35 61.1429

1 36 51.5417

1.5 34 46.1618

Test statistic = 4.2991 P-Value = 0.116537

The Kruskal-Wallis test tests the null hypothesis that the medians of Recovery within each of the 3

levels of Concentration are the same. The data from all the levels is first combined and ranked from

smallest to largest. The average rank is then computed for the data at each level. Since the P-

value is greater than 0.05, there is not a statistically significant difference amongst the medians at

the 95.0% confidence level.

4.2.2. DiFi potency assay

The aim of this section is to analyze if the results obtained with Concentration (0.5. 1.0 and 1.5) are

significant different or in other words to determine whether or not the Concentration (0.5. 1.0 and

1.5) has an impact on the Recovery for the DiFi potency assay.

An ANalysis Of VAriance (Anova) is used to analyze the relationships between different

Concentration (0.5. 1.0 and 1.5) and the Recovery obtained. It compares the three Concentrations

in order to see if any of the concentration means is statistically different from the others in the DiFi

potency assay.

The Kolmogorov-Smirnov Test is a goodness of fit tests for residual. It determines whether

Residual can be adequately modelled by a normal distribution.

Kolmogorov-Smirnov Test

Normal

DPLUS 0.102855

DMINUS 0.0514361

DN 0.102855

P-Value 0.175569

Since the smallest P-value amongst the tests performed is greater than 0.05, we can not reject the

idea that Residual comes from a normal distribution with 95% confidence.

Page 169: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

169

Histogram for Residual

-0,26 -0,06 0,14 0,34 0,54

Residual

0

10

20

30

40

50

fre

qu

en

cy

Distribution

Normal

The statistic displayed in this table tests the null hypothesis that the standard deviations of

Recovery within each of the 3 levels of Concentration is the same. Of particular interest is the P-

value. Since the P-value is less than 0.05, there is a statistically significant difference amongst the

standard deviations at the 95.0% confidence level. This violates one of the important assumptions

underlying the analysis of variance and will invalidate the statistical tests.

Variance Check

Test P-Value

Cochran's C 0.567348 0.00059957

Bartlett's 1.18186 0.0000964052

This table shows the mean Recovery for each level of Concentration. It also shows the standard

error of each mean, which is a measure of its sampling variability. The standard error is formed by

dividing the standard deviation at each level by the square root of the number of observations at

that level. The table also displays an interval around each mean. The intervals currently displayed

are 95.0% confidence intervals for each mean separately. 95.0% of such intervals will contain the

true means.

Table of Means for Recovery by Concentration with 95.0 percent confidence intervals

Stnd. error

Concentration Count Mean (individual) Lower limit Upper limit

0.5 40 0.97975 0.0253103 0.928555 1.03095

1 38 0.959684 0.0125334 0.934289 0.985079

1.5 37 1.011 0.019152 0.972158 1.04984

Total 115 0.983174

Page 170: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

170

0,5

1

1,5

Box-and-Whisker Plot

0,75 0,95 1,15 1,35 1,55

Recovery

Co

nce

ntr

ati

on

This graph shows 3 box-and-whisker plots, one for each level of Concentration. The rectangular

part of the plot extends from the lower quartile to the upper quartile covering the center half of each

sample. The center lines within each box show the location of the sample medians. The plus signs

indicate the location of the sample means. The whiskers extend from the box to the minimum and

maximum values in each sample except for any outside or far outside points, which will be plotted

separately. Outside points are points which lie more than 1.5 times the interquartile range above or

below the box and are shown as small squares. Far outside points are points which lie more than

3.0 times the interquartile range above or below the box and are shown as small squares with plus

signs through them. In this case, there are 4 outside points.

Therefore, it is strongly recommended when the result of a test is so sensitive to outliers the use of

the less sensitive test. In this case a test on the medians has been chosen (Kruskal-Wallis Test)

which compares medians instead of means.

Kruskal-Wallis Test for Recovery by Concentration

Concentration Sample Size Average Rank

0.5 40 53.0375

1 38 54.6184

1.5 37 66.8378

Test statistic = 3.87707 P-Value = 0.143915

The Kruskal-Wallis test tests the null hypothesis that the medians of Recovery within each of the 3

levels of Concentration are the same. The data from all the levels is first combined and ranked from

smallest to largest. The average rank is then computed for the data at each level. Since the P-

value is greater than 0.05, there is not a statistically significant difference amongst the medians at

the 95.0% confidence level.

Page 171: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

171

4.2.3. Conclusions

The Variance Check shows that there is a statistically significant difference amongst the standard

deviations at the 95.0% confidence level both for the CTLL-2 and DiFi potency assays. This

violates one of the important assumptions underlying the ANalysis Of VAriance and invalidates the

statistical tests. Therefore the ANOVA can not be performed. In this case, the presence of outside

points suggests to use a more robust test which compares medians instead of means (Kruskal-

Wallis Test) and the result is that there is not a statistically significant difference amongst the

medians at the 95.0% confidence level.

Summary Table for Concentration

Comments

YES NO

Assay 1

Test for normality KS Test P-Value=0.17. The observation can be adequately

modeled by a normal distribution

Variance CheckCochran's and Bartlett's P-Value < 0.05.There is a

statistically significant difference amongst the standard

deviations

Test on Medians : Kruskal-

Wallis Test Kruskal-Wallis Test P-Value=0.12. There is not a

statistically significant difference amongst the medians

Assay 2

Test for normality KS Test P-Value=0.17. The observation can be adequately

modeled by a normal distribution

Variance CheckCochran's and Bartlett's P-Value < 0.05.There is a

statistically significant difference amongst the standard

deviations

Test on Medians : Kruskal-

Wallis Test Kruskal-Wallis Test P-Value=0.14. There is not a

statistically significant difference amongst the mediansKS=Kolmogorov-Smirnov

P-value > 0.05

Results of the analyses by Concentration

4.3. Results of the analyses by Range

4.3.1. CTLL-2 potency assay

The aim of this section is to analyze if the results obtained with Range (5-30ng/mL, 0.75-100ng/mL

and 6.8-80ng/mL) are significant different or in other words to determine whether or not the Range

(5-30ng/mL, 0.75-100ng/mL and 6.8-80ng/mL) has an impact on the Recovery for the CTLL-2

potency assay.

An ANalysis Of VAriance (Anova) is used to analyze the relationships between different Range (5-

30ng/mL, 0.75-100ng/mL and 6.8-80ng/mL) and the Recovery obtained. It compares the three

Ranges in order to see if any of the Range means is statistically different from the others in the

CTLL-2 potency assay.

The Kolmogorov-Smirnov Test is a goodness of fit tests for residual. It determines whether

Residual can be adequately modelled by a normal distribution.

Page 172: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

172

Kolmogorov-Smirnov Test

Normal

DPLUS 0.120484

DMINUS 0.0580533

DN 0.120484

P-Value 0.0948716

Since the smallest P-value amongst the tests performed is greater than 0.05. We can not reject the

idea that Residual comes from a normal distribution with 95% confidence.

Histogram for Residual

-0,29 -0,09 0,11 0,31 0,51

Residual

0

10

20

30

40

50

fre

qu

en

cy

Distribution

Normal

The statistics displayed in these tables test the null hypothesis that the standard deviation of

Recovery within each of the 3 levels of Range is the same. Of particular interest are the P-values.

Since the greater P-value is less than 0.05, there is a statistically significant difference amongst the

standard deviations at the 95.0% confidence level. This violates one of the important assumptions

underlying the analysis of variance and will invalidate the statistical tests.

Variance Check

Test P-Value

Cochran's C 0.506552 0.017787

Bartlett's 1.15402 0.00075371

This table shows the mean Recovery for each level of Range. It also shows the standard error of

each mean, which is a measure of its sampling variability. The standard error is formed by dividing

the standard deviation at each level by the square root of the number of observations at that level.

The table also displays an interval around each mean. The intervals currently displayed are 95.0%

confidence intervals for each mean separately. 95.0% of such intervals will contain the true means.

Page 173: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

173

Table of Means for Recovery by Range with 95.0 percent confidence intervals

Stnd. error

Range Count Mean (individual) Lower limit Upper limit

(0.75-100ng/mL) 41 1.00066 0.014348 0.97166 1.02966

(5-30ng/mL) 18 1.07111 0.0329012 1.0017 1.14053

(6.8-80ng/mL) 46 1.045 0.0249638 0.99472 1.09528

Total 105 1.03216

(0.75-100ng/mL)

(5-30ng/mL)

(6.8-80ng/mL)

Box-and-Whisker Plot

0,75 0,95 1,15 1,35 1,55

Recovery

Ra

ng

e

This graph shows 3 box-and-whisker plots, one for each level of Range. The rectangular part of

the plot extends from the lower quartile to the upper quartile, covering the center half of each

sample. The center lines within each box show the location of the sample medians. The plus signs

indicate the location of the sample means. The whiskers extend from the box to the minimum and

maximum values in each sample, except for any outside or far outside points, which will be plotted

separately. Outside points are points which lie more than 1.5 times the interquartile range above or

below the box and are shown as small squares. Far outside points are points which lie more than

3.0 times the interquartile range above or below the box and are shown as small squares with plus

signs through them. In this case, there is 1 outside point.

Therefore, it is strongly recommended when the result of a test is so sensitive to one observation

the use of the less sensitive test. In this case, a test on the medians has been chosen (Kruskal-

Wallis Test) which compares medians instead of means.

Kruskal-Wallis Test for Recovery by Range

Range Sample Size Average Rank

(0.75-100ng/mL) 41 47.5

(5-30ng/mL) 18 61.7222

(6.8-80ng/mL) 46 54.4891

Test statistic = 2.92379 P-Value = 0.231797

Page 174: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

174

The Kruskal-Wallis tests the null hypothesis that the medians of Recovery within each of the 3

levels of Range are the same. The data from all the levels is first combined and ranked from

smallest to largest. The average rank is then computed for the data at each level. Since the P-

value is greater than 0.05, there is not a statistically significant difference amongst the medians at

the 95.0% confidence level.

4.3.2. DiFi potency assay

The aim of this section is to analyze if the results obtained with Range (5-30ng/mL, 0.75-100ng/mL

and 6.8-80ng/mL) are significant different or in other word, to determine whether or not the Range

(5-30ng/mL, 0.75-100ng/mL and 6.8-80ng/mL) has an impact on the Recovery for the DiFi potency

assay.

An ANalysis Of VAriance (Anova) is used to analyze the relationships between different Range (5-

30ng/mL, 0.75-100ng/mL and 6.8-80ng/mL) and the Recovery obtained. It compares the three

Ranges in order to see if any of the Range means is statistically different from the others in The

DiFi potency assay.

The Kolmogorov-Smirnov Test is a goodness of fit tests for residual. It determines whether

Residual can be adequately modelled by a normal distribution.

Kolmogorov-Smirnov Test

Normal

DPLUS 0.15246

DMINUS 0.058621

DN 0.15246

P-Value 0.0095328

Since the smallest P-value amongst the tests performed is less than 0.05, we can reject the idea

that Residual comes from a normal distribution with 95% confidence.

Histogram for Residual

-0,3 -0,1 0,1 0,3 0,5 0,7 0,9

Residual

0

10

20

30

40

50

fre

qu

en

cy

Distribution

Normal

Page 175: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

175

The statistic displayed in this table tests the null hypothesis that the standard deviations of

Recovery within each of the 3 levels of Range is the same. Of particular interest is the P-value.

Since the P-value is greater than 0.05, there is not a statistically significant difference amongst the

standard deviations at the 95.0% confidence level.

Variance Check

Test P-Value

Levene's 0.89453 0.4117

The ANOVA table decomposes the variance of Recovery into two components: a between-group

component and a within-group component. The F-ratio, which in this case equals 0.461729, is a

ratio of the between-group estimate to the within-group estimate. Since the P-value of the F-test is

greater than 0.05, there is not a statistically significant difference between the mean Recovery from

one level of Range to another at the 95.0% confidence level.

ANOVA Table for Recovery by Range

Source Sum of Squares Df Mean Square F-Ratio P-Value

Between groups 0.0143836 2 0.00719182 0.46 0.6314

Within groups 1.74449 112 0.0155758

Total (Corr.) 1.75888 114

(0.25-95nM) (2-12nM) (5-55nM)

Means and 95,0 Percent Confidence Intervals (internal s)

Range

0,87

0,9

0,93

0,96

0,99

1,02

1,05

Re

co

ve

ry

This table shows the mean Recovery for each level of Range. It also shows the standard error of

each mean, which is a measure of its sampling variability. The standard error is formed by dividing

the standard deviation at each level by the square root of the number of observations at that level.

The table also displays an interval around each mean. The intervals currently displayed are 95.0%

confidence intervals for each mean separately. 95.0% of such intervals will contain the true means.

Page 176: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

176

Table of Means for Recovery by Range with 95.0 percent confidence intervals

Stnd. error

Range Count Mean (individual) Lower limit Upper limit

(0.25-95nM) 47 0.98834 0.0184397 0.951223 1.02546

(2-12nM) 18 0.957222 0.0369164 0.879335 1.03511

(5-55nM) 50 0.98766 0.015549 0.956413 1.01891

Total 115 0.983174

(0.25-95nM) (2-12nM) (5-55nM)

Residual Plot for Recovery

-0,6

-0,4

-0,2

0

0,2

0,4

0,6

res

idu

al

Range

4.3.3 Conclusions

The Variance Check shows that there is a statistically significant difference amongst the standard

deviations at the 95.0% confidence level for the CTLL-2 potency assay. This violates one of the

important assumptions underlying the ANOVA and invalidates the statistical tests. Therefore the

ANOVA can not be performed. In this case, the presence of outside points suggests using a more

robust test which compares medians instead of means (Kruskal-Wallis Test) and the result is that

there is not a statistically significant difference amongst the medians at the 95.0% confidence level.

As for the DiFi potency assay, the ANOVA shows that there is not a significant statistically

difference between the means from one level of Range to another at the 95.0% confidence level.

Page 177: DEVELOPMENT OF INNOVATIVE BIOASSAY PRINCIPLES FOR

177

Summary Table for Range

Comments

YES NO

Assay 1

Test for normality KS Test P-Value=0.09. The observation can be adequately

modeled by a normal distribution

Variance CheckCochran's and Bartlett's P-Value < 0.05.There is a

statistically significant difference amongst the standard

deviations

Test on Medians : Kruskal-

Wallis Test Kruskal-Wallis Test P-Value=0.23. There is not a

statistically significant difference amongst the medians

Assay 2

Test for normality KS Test P-Value=0.009. The observation can't be

adequately modeled by a normal distribution

Variance Check Levene's P-Value=0.41.There is not a statistically

significant difference amongst the standard deviations

Test on Means: ANOVA ANOVA P-Value=0.63. There is not a statistically

significant difference between the meansKS=Kolmogorov-Smirnov

P-value > 0.05

Results of the analyses by Range

5. Analysis on failure rates

In order to verify whether there is a significant difference in the failure rates (FR) between the

different calculation models or not, the results have been summarized in the following table.

PL 4PL 5PL Total

Assay1

Number of failures 0 10 11 21

Number of observations 54 36 36 126

Failure rate [%] 0 27,78 30,56 16,67

Assay2

Number of failures 0 5 6 11

Number of observations 54 36 36 126

Failure rate 0 13,89 16,67 8,73

Total

Number of failures 0 15 16 31

Number of observations 108 72 72 252

Failure rate 0 20,83 22,22 12,30

It is clear from the simple observation of the failure rates that there is a significant difference

between PL and the other models (4PL and 5PL) in both assays. This difference is greater if only

the results of the CTLL-2 potency assay (Assay 1) are taken into account.

In any case, statistical tests have been performed separately for the CTLL-2 potency assay (Assay

1) and the DiFi potency assay (Assay 2).

The Hypothesis is that the failure rate is the same for the three models and that it is equal to the

mean value (16.67% for the CTLL-2 potency assay and 8.73% for the DiFi potency assay).

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5.1 CTLL-2 potency assay

Hypothesis Tests: PL Failure rate = 0.16667

Sample proportion = 0.0

Sample size = 54

Approximate 95.0% confidence interval for p: [0.0; 0.0660315]

The two hypotheses to be tested are:

Null Hypothesis: PL Failure rate = 0.16667

Alternative: not equal

P-Value = 0.000105962

Reject the null hypothesis for alpha = 0.05.

In this sample of 54 observations, the sample proportion equals 0.0. Since the P-value for the test

is less than 0.05, the null hypothesis is rejected at the 95.0% confidence level. The confidence

interval shows that the values of theta supported by the data fall between 0.0 and 0.0660315.

Hypothesis Tests 4PL Failure rate = 0.16667

Sample proportion = 0.27778

Sample size = 36

Approximate 95.0% confidence interval for p: [0.142004; 0.451864]

The two hypotheses to be tested are:

Null Hypothesis: 4PL Failure rate = 0.16667

Alternative: not equal

P-Value = 0.130431

Do not reject the null hypothesis for alpha = 0.05.

In this sample of 36 observations, the sample proportion equals 0.27778. Since the P-value for the

test is greater than or equal to 0.05, the null hypothesis cannot be rejected at the 95.0% confidence

level. The confidence interval shows that the values of theta supported by the data fall between

0.142004 and 0.451864.

Hypothesis Tests 5PL Failure rate = 0.16667

Sample proportion = 0.30556

Sample size = 36

Approximate 95.0% confidence interval for p: [0.163477; 0.481075]

The two hypotheses to be tested are:

Null Hypothesis: 5PL Failure rate = 0.16667

Alternative: not equal

P-Value = 0.0569794

Do not reject the null hypothesis for alpha = 0.05.

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In this sample of 36 observations, the sample proportion equals 0.30556. Since the P-value for the

test is greater than or equal to 0.05, the null hypothesis cannot be rejected at the 95.0% confidence

level. The confidence interval shows that the values of theta supported by the data fall between

0.163477 and 0.481075.

5.2 DiFi potency assay

Hypothesis Tests: PL Failure rate = 0.0873

Sample proportion = 0.0

Sample size = 54

Approximate 95.0% confidence interval for p: [0.0; 0.0660315]

The two hypotheses to be tested are:

Null Hypothesis: PL Failure rate = 0.0873

Alternative: not equal

P-Value = 0.0144127

Reject the null hypothesis for alpha = 0.05.

In this sample of 54 observations, the sample proportion equals 0.0. Since the P-value for the test

is less than 0.05, the null hypothesis is rejected at the 95.0% confidence level. The confidence

interval shows that the values of theta supported by the data fall between 0.0 and 0.0660315.

Hypothesis Tests: 4PL Failure rate = 0.0873

Sample proportion = 0.13889

Sample size = 36

Approximate 95.0% confidence interval for p: [0.0466783; 0.294976]

The two hypotheses to be tested are:

Null Hypothesis: 4PL Failure rate = 0.0873

Alternative: not equal

P-Value = 0.404229

Do not reject the null hypothesis for alpha = 0.05.

In this sample of 36 observations, the sample proportion equals 0.13889. Since the P-value for the

test is greater than or equal to 0.05, the null hypothesis cannot be rejected at the 95.0% confidence

level. The confidence interval shows that the values of theta supported by the data fall between

0.0466783 and 0.294976.

Hypothesis Tests: 5PL Failure rate = 0.0873

Sample proportion = 0.16667

Sample size = 36

Approximate 95.0% confidence interval for p: [0.0637223; 0.32812]

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The two hypotheses to be tested are:

Null Hypothesis: 5PL Failure rate = 0.0873

Alternative: not equal

P-Value = 0.179011

Do not reject the null hypothesis for alpha = 0.05.

In this sample of 36 observations, the sample proportion equals 0.16667. Since the P-value for the

test is greater than or equal to 0.05, the null hypothesis cannot be rejected at the 95.0% confidence

level. The confidence interval shows that the values of theta supported by the data fall between

0.0637223 and 0.32812.

5.3 Conclusions

The statistical tests confirm that there is a statistically significant difference between the failure rate

of PL and the failure rates of the others (4PL and 5PL).

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ABSTRACT

Keywords: Bioassay, quality control, analysis models, read-out systems, STAT5 phosphorylation

assay, Interleukin-7

The quality of biopharmaceuticals is usually monitored by using biological assays. The aim of this

study was to optimize existing methods for biological assays and to implement alternative assay

formats. First, analysis models and read-out systems for proliferation assays, which are frequently

applied for quality control purposes, were compared.

Regarding the comparison of analysis models, the parallel line model was compared to the logistic

models four- and five-parameter fit. The results of this comparison revealed a slightly better

accuracy and precision of the logistic models in comparison to the parallel line model; however

differences were not statistically significant different. On the other side, the logistic models showed

a significantly higher failure rate.

Regarding the comparison of read-out systems, it was tested in this study, whether luminescence

or fluorescence systems could be of advantage in comparison to the colorimetric system, originally

in use for detection of the response of proliferation assays at Merck Serono. From the results of

this study, it can be concluded that the luminescence technique seems to be the most

advantageous of the three read-outs for potency assays. It is extremely sensitive, therefore leading

to cell savings and provides the highest signal to noise ratios, leading to very precise results.

Moreover, it is the fastest of the three methods for all assays investigated (CTLL-2, DiFi and Kit

225 potency assay), since the plate can already be measured 5 - 10min after addition of substrate.

As an alternative to the commonly used proliferation assays, an intracellular phosphorylation assay

was developed for a cytokine fusion protein including Interleukin (IL)-7, since the originally used

proliferation assay suffered from a very long incubation time and a poor robustness. Using western

blotting, STAT5 was identified as a target for development of this assay. This study was further

expanded to a comparison of IL-7 signaling in different cell lines (Kit 225, PB-1 and 2E8) and to a

comparison between the signaling pathways of the two γc cytokines IL-7 and IL-2. The study

showed that some of the investigated targets were induced by IL-2 stimulation only, and not by IL-7

stimulation. Regarding the comparison between the different cell lines, interesting differences in the

expression pattern and kinetics of activation by IL-7 could be observed. However, in this study, the

only pathway identified to be activated in all three cell lines by IL-7, was the STAT5 pathway and

the associated induction of pim-1, making STAT5 a suitable target for development of the

phosphorylation assay and the IL-7 signal transduction cascade an interesting target for further

explorations.

The developed STAT5 phosphorylation assay showed very accurate and precise results. The main

advantage of this assay are its rapidness - reducing the total time of the assay from six to three

days – and the higher robustness in comparison to the proliferation assay. It can serve as a fast

and reliable alternative to classical end-point assays and is well-suited for use in quality control of

biopharmaceuticals.

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ZUSAMMENFASSUNG

Stichworte: Bioassay, Qualitätskontrolle, Auswertemodelle, Read-out Systeme, STAT5

Phosphorylierungsassay, Interleukin-7

Die Qualität von Biopharmazeutika wird üblicherweise durch Bioassays kontrolliert. Das Ziel dieser

Arbeit war, bestehende Methoden für Bioassays zu optimieren und alternative Assayformate zu

implementieren. Zunächst wurden Auswertemethoden und Read-out Systeme für

Proliferationsassays, die häufig für Qualitätskontrollzwecke eingesetzt werden, miteinander

verglichen.

Hinsichtlich des Vergleichs von Auswertemodellen wurde das Parallel Line Model mit den beiden

logistischen Modellen, Vier- und Fünf-Parameter Fit verglichen. Die Ergebnisse dieser Studie

zeigten eine etwas höhere Genauigkeit und Präzision der logistischen Modelle im Vergleich zum

Parallel Line Model; die Unterschiede waren jedoch statistisch nicht signifikant. Andererseits waren

die Fehlerraten der logistischen Modelle signifikant höher.

Für den Vergleich verschiedener Read-out Systeme wurde in dieser Studie getestet, ob

Lumineszenz oder Fluoreszenz Systeme vorteilhaft gegenüber dem kolorimetrischen System sind,

das bei Merck Serono ursprünglich für die Detektion der Antwort von Proliferationsassays

verwendet wurde. Aus den Ergebnissen dieser Studie kann geschlussfolgert werden, dass die

Lumineszenztechnik die vielversprechendste der drei Read-out Methoden für Bioassays ist. Sie ist

extrem sensitiv und mindert somit den Verbrauch an Zellen, liefert die höchsten Signal-Rausch-

Verhältnisse und führt zu sehr präzisen Resultaten. Außerdem ist sie die schnellste der drei

Methoden für alle untersuchten Assays (CTLL-2, DiFi und Kit 225 Assay), da die Platte bereits 5 -

10min nach Substratzugabe gemessen werden kann.

Als Alternative zu den allgemein verwendeten Proliferationsassays wurde ein intrazellulärer

Phosphorylierungsassay für ein Zytokinfusionsprotein mit Interleukin (IL)-7 Anteil entwickelt, da die

Inkubationszeit des ursprünglichen Proliferationsassays sehr lang war und die Robustheit des

Assays nicht angemessen war. Mittels Westernblotanalyse wurde STAT5 als Target für diesen

Assay identifiziert. Diese Studie wurde ausgeweitet zu einem Vergleich der IL-7

Signaltransduktionswege in verschiedenen Zelllinien (Kit 225, PB-1 und 2E8) und zu einem

Vergleich der Signaltransduktionswege der beiden γc Zytokine, IL-7 und IL-2. Die Ergebnisse der

Studie zeigten, dass einige der untersuchten Targets nur durch IL-2 Stimulation und nicht durch IL-

7 Stimulation induziert wurden. In den verschiedenen Zelllinien konnten interessante Unterschiede

der Expressionsmuster und Aktivierungskinetiken durch IL-7 beobachtet werden. Jedoch war der

einzige, identifizierbare Signaltransduktionsweg, der in dieser Studie durch IL-7 aktiviert wurde, der

STAT5 Signalweg und die damit verbundene Induktion von Pim-1. Dies machte STAT5 zu einem

geeigneten Target für die Entwicklung eines Phosphorylierungsassays und die IL-7

Signaltransduktionskaskade zu einem interessanten Ziel für weitere Untersuchungen.

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Der entwickelte STAT5 Phosphorylierungsassay zeigte sehr genaue und präzise Ergebnisse. Die

wesentlichen Vorteile dieses Assays sind seine Schnelligkeit – da die Gesamtdauer des Assays

von sechs auf drei Tage reduziert werden konnte – und die höhere Robustheit im Vergleich zum

Proliferationsassay. Er ist somit eine schnelle und zuverlässige Alternative im Vergleich zu den

klassischen Proliferationsassays und ist gut geeignet für die Qualitätskontrolle von

Biopharmazeutika.

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CURRICULUM VITAE Persönliche Daten

Name: Cornelia Andrea Zumpe

Geburtsdatum/-Ort: 06.02.1983 in Nürnberg

Familienstand: ledig

Staatsangehörigkeit: deutsch

Anschrift: Martin-Gnad-Str. 45, 90427 Nürnberg

Schulbildung

1989 – 1993 Grundschule Großgründlach

1993 – 2002 Wilhelm-Löhe-Schule Nürnberg

Jun 2002 Allgemeine Hochschulreife

Hochschulbildung

Okt 2002 – Sep 2005 Bachelorstudium „Molecular Science“ (B.Sc.)

Universität Erlangen-Nürnberg

Thema der Bachelorarbeit: „Einfluss des Protein-

/Hilfsstoffverhältnisses auf die Stabilität von Katalase bei der

Sprühtrocknung“

Okt 2005 – Mai 2007 Masterstudium „Molecular Life Science“ (M.Sc.)

Universität Erlangen-Nürnberg

Nov 2006 – Apr 2007 Masterarbeit am „Institut Polytechnique LaSalle Beauvais“

Thema: „Analysis of protein adducts formed during thermal

treatment of infant formulas by GC-MS/MS“

Wissenschaftliche Tätigkeit

Aug 2007 - dato Wissenschaftliche Tätigkeit bei der Firma Merck Serono, in

Kooperation mit der FAU Erlangen-Nürnberg (Institut für

Lebensmittelchemie)

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Eidesstaatliche Erklärung gem. § 4.2 und 4.6 der Promotionsordnung der Naturwissenschaftlichen

Fakultät der Friedrich-Alexander-Universität Erlangen-Nürnberg.

Ich erkläre hiermit, dass ich die vorliegende Arbeit ohne fremde Hilfe angefertigt und nur die im

Literaturverzeichnis angeführten Quellen und Hilfsmittel verwendet habe.

Desweiteren erkläre ich hiermit, dass ich an keiner anderen Stelle ein Prüfungsverfahren

beantragt, bzw. die Dissertation in dieser oder einer anderen Form bereits anderweitig als

Prüfungsarbeit verwendet oder einer anderen Fakultät als Dissertation vorgelegt habe.

Ort, Datum Unterschrift