actinide chemistry and repository science program in ......ans 14th biennial topical meeting la-ur...

ANS 14th Biennial Topical Meeting LA-UR 05-9615 Carlsbad April 3-6 2006

Actinide Chemistry and Repository Science Program in support of the Waste Isolation

Pilot Plant (WIPP)

J-F Lucchini M Borkowski MK Richmann and DT Reed

Los Alamos National Laboratory EES Carlsbad Operations


DOE weapons complex The WIPP is located in southeastern New Mexico 26 miles east of Carlsbad Waste disposal operations began on March 26 1999

The Waste Isolation Pilot Plant WIPP a cornerstone of the DOE s cleanup effort is designed to permanently dispose of defense-generated transuranic radioactive waste from research and production activities in the


Transuranic waste is shipped to the WIPP from many generator and storage sites such as Savannah River Site Oak Ridge Argonne Rocky Flat Idaho Nevada Test Site Livermore and Los Alamos All shipments are done using specially designed TRUPAC-II containers


Disposal rooms are excavated in an ancient stable salt formation 2150 feet (almost one-half mile) underground Transuranic waste which consists of clothing tools rags debris andother disposable items contaminated with radioactive elements mostly plutonium are emplaced in 55 gallon steel drums for permanent disposal


Waste and magnesium oxide are placed in a WIPP Disposal Room On March 23 2006 the amount of 76156 containers are disposed in the underground


Center an institute that is operated by New Mexico State University Our most important purpose is to provide laboratory research andprogram support on actinide-related issues to the DOE Carlsbad Field Office (CBFO) to maintain the certification of the WIPP Additionally we have the capability to conduct research programs in actinide environmental chemistry for other sponsors

The Actinide Chemistry and Repository Science Program (ACRSP) is part of a larger multi-disciplinary Los Alamos group (EES-12) working in Carlsbad We conduct our laboratory research programs at the Carlsbad Environmental Monitoring and Research


Glove boxes with controlled atmosphere


Glove box for high radioactivity operation and LCS (behind)


Hoods for work with low radioactivity samples


ICP-MS and Dr Mike Richmann as operator


Lab Capability

ICP-MS designated for Pu and AmPhoto-acoustic spectroscopy with powerful laserXRD (x-ray diffraction)Spectroscopy (Cary 500)Ion ChromatographyCO2 analysis (down to ppb level)Liquid Scintillation CountingGlove boxes with controlled atmosphere (lt01 ppm O2)


The Actinide Chemistry and Repository Science Program (ACRSP) is conducted according to five Test Plans approved by CBFO

SolubilityStability of Uranium (VI) in WIPPbull Solubility of U(VI) in WIPP brine bull Redox stability of U(VI) in WIPP brine bull Effect of radiolytic products on uranium

speciation

Plutonium (VI) Reduction by Ironbull Limited scope - confirmatory study on effect of various

form of iron iron oxide on plutonium redox reaction


Neodymium (III) Solubility in WIPP Brinebull Solubility of Nd(III) in WIPP brine an analog for

Am(III) and Pu(III) studied as a function of pCH+and carbonate concentration and measured from over-saturation and under-saturation

Americium SolubilityStability in WIPP Brinebull Solubility of Am(III) in WIPP brine

bull Effect of radiolytic products and repository components on americium oxidation and stabilitysolubility of Am higher oxidation states at the repository conditions


Plutonium Speciation and Solubility in the WIPPbull Technical assessment of the current WIPP

Database on Pubull Relevance of Pu(III) in the WIPPbull Solubility of Pu(IV) in the WIPPbull Reduction of Pu(V0 and Pu(VI) in the WIPPbull Speciation of plutonium in the WIPP


1 Effect of radiolytic products of brine microbial activity and repository components on redox speciation of plutonium americium and uranium

2 Solubility of transuranium elements in WIPP brine (effect of pCH+ carbonate organic ligands etc)

Two major programmatic groups can be distinguished


Brine Composition Used in Actinide Solubility StudiesERDA-6 GWB MgCl2simplified

NaCl simplified

Component gL ML gL ML gL ML gL MLNaCl 2486 4254 1678 2874 2922 50

MgCl26H2O 3667 0018 1934 0953 7519 3704

Na2SO4 2252 0159 2361 0166

NaBr 1074 0010 2565 0025Na2B4O710H2O 57 0015 1403 0037

KCl 6869 0092 3257 0437

LiCl - - 0174 0004

CaCl22H2O 1672 0011 1896 0013

Ionic strength 4965 M 6839 M 111 M 50 MDensity gmL 1183 1216 1252 1185

GWB - Generic Weep BrineERDA-6 - Energy Research and Development Administration Well 6


Stability of H2O2 and OCl- in brine

0 20 40 60 80 100 120 140 160 18000

01

02

03

04

05

06

07

08

09

Abs

orba

nce

at 3

51 n

m

Time hours

GWB at pcH = 85 y = 0836e-0012t

ERDA-6 at pcH = 90 y = 0789e-0075t

Decomposition of H2O2 in brine

250 275 300 325 350 375 400

000

002

004

006

008

010

012

014

016

Abs

orba

nce

(rel

uni

t)Wavelength (nm)

t=0h t=6h t=12h t=18h t=24h t=30h t=36h t=42h t=48h t=54h t=60h t=66h

OCl- in 5 M NaCl

2 OCl- + H2O2 2 Cl- + H2O + O2

OCl- + Br- Cl- + OBr- + hellip


Dependence of hypochlorite generation as a function of absorbed dose of α radiation and NaCl concentration

0 100 200 300 400 500 6000000

0001

0002

0003

0004

0005

0006

5 m NaCl

4 m NaCl

3 m NaCl

2 m NaCl

H

ypoc

hlor

ite C

once

ntra

tion

M

Dose (kGy)


Primary G-values calculated for different chloride concentrations

0 1 2 3 4 5 6 7 8 9 10 11 12 13000

001

002

003

004

005

006

Hyp

ochl

orite

Sat

urat

ion

M

238Pu Activity CiL

5 M NaCl

0380402044032305002740550235

GClOHGH2O2

Cl-concentration

[M]

Kelm M I Pashalidis IJ Kim Applied Radiation and Isotopes 51 (1999) 637-642


The presence of Fe0 and Fe2+ resulted in the rapid loss of plutonium from solution In the case of ferric oxide some loss of Pu was noted but residual concentrations remained high and it was (postulated) due to sorption not reductionprecipitation The most complete and rapid loss of Pu occurred for magnetite which was the only iron phase that contained Fe2+ These results show that Fe0 and Fe2+ effectively remove dissolved plutonium from brine

0 100 200 300 400 500 600

0

1x10-5

2x10-5

3x10-5

4x10-5

5x10-5

Pu

conc

entra

tion

MTime in hours

Ferric oxide

Fe Powder

Fe Coupon

Magnetite

Reduction of Pu(VI) by Iron and Iron Oxides

Effect of various forms of iron on plutonium (VI) reduction in ERDA-6 brine at pCH+=92 and anoxic conditions


The absorption spectrum of the plutonium in GWB brine Since the pH is ~ 9 the plutonium is hydrolyzed (complexed with hydroxide) resulting in a 20 nm shift in the absorption maximum to 851 nm The absorption spectrum of this solution was stable over the three-month period that it was monitored

300 400 500 600 700 800 900

000

002

004

006

008

010

Opt

ical

Den

sity

Wavelength (nm)

Pu(VI) in GWB Brine

Peak at 851 nm is hydrolyzed Pu(VI)


Solubility of Nd(III) and U(VI)The goal of this research is to provide the experimental data for the solubility of trivalent and hexavalent actinides

In this study neodymium (III) was used as a redox-invariant analog for Am (III) and Pu (III)

The experiments in each approach are conducted in GWB and ERDA-6 as a function of pCH+ and carbonate concentration

Simplified brine 5 M NaCl was used for comparison


Experimental limitations

The highest concentration of carbonate ion in GWB and ERDA-6 brine before the cloud point was observed was determined to be 2- 4 x 10-2 M

The highest pCH+ before the cloud point was observed was - for Erda-6 was equal to 108 - for GWB brine was equal to 87


00 05 10 15 20 250

2

4

6

8

10

0 2 40

2

4

pH re

adin

g

Volume of 100 M HCl mL

BaseAcid Titration in ERDA-6 Brine

Buffering by borate

Buffering by sulfate

pH re

adin

g

pCH+ calculated

pH reading vs pcH for HP water

pHread = 09998 pcH - 09438

Low pCH+ limit and pCH+ vs pH reading in ERDA-6 brine


Low pCH+ limit and pCH+ vs pH reading in GWB brine

00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g


BaseAcid Titration in GWB Brine

Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6

bull pCH+ range 75 ndash 12

bull Initial carbonate concentrations

0 (carbonate free) 10-5 10-4 10-3 and 10-2 M

bull NdCl3 solution was used as a spike in the over-saturation approach

bull Initial Nd(III) concentration was 5x10-5 M and U(VI) was 17x10-5 M


ERDA-6 cont

bull NdOH(CO3) solid prepared in our lab was used in the under-saturation approach with carbonate

bull Nd(OH)3 solid commercial from Alfa Aesar was used in the under-saturation approach without carbonate

bull All carbonate free experiments were conducted in the nitrogen glove box and carbonate ion was removed from the brine prior to the experiment


0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M

Equilibration Time days

ERDA-6kinetic of equilibration

oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

- oversaturation - undersaturation - trend

Nd

Con

cent

ratio

n M

pCH+

ERDA-6carbonate free system

over- and under-saturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+

over- under- carbonate - 10-2 M - 10-3 M - 10-4 M - 10-5 M

- trend (no carb)

ERDA-6over- and under-saturation

with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2

uranium detection limit

Ura

nium

con

cent

ratio

n M

Time Days

pCH+=8 pCH+=9 pCH+=10 pCH+=11 pCH+=12

ERDA-6 carbonate free

U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+

air atmosphere nitrogen atmosphere

initial uranium concentration

U (VI)


GWBbull pCH+ range 65 ndash 85




bull Initial Nd(III) concentration was 5x10-5 M


GWB CONT


bull Nd(OH)3 solid commercial from Alfa Aesar was used in under-saturation approach without carbonate



60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+

over- under- carbonate - 10-2 M - 10-3 M - 10-4 M - 10-5 M - trend

GWBover- and under-saturation

with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+

- oversaturation - undersaturation - carbonate trend


carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days

pCH+=6 pCH+=7 pCH+=8 pCH+=9

GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+

GWBcarbonate free over-saturation


5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+


5 M NaClover- and under-saturation

carbonate free

Nd (III)


ConclusionsThe solubility experiments are still going on but preliminary conclusions can be madeThe trend in Nd(III) solubility measured as a function of pCH+ in 5 M NaCl is in good agreement with literature data however measured solubility is slightly higher than those reported in lower concentrations of NaCl Nd(III) and U(VI) solubilities are greater in GWB brine than in ERDA-6 brine The neodymium data obtained from over-saturation experiments is very close to data obtained from under-saturation experiments It means that in many cases a steady state was achievedAlmost no effect of carbonate on Nd(III) solubility was observed


ConclusionsThe following Nd(III) solubilities at pCH+ = 85 were measured

With carbonate No carbonate ERDA-6 2 x 10-8 M 4 x 10-8 MGWB 3 x 10-7 M 3 x 10-7 M

Calculated Estimated with Estimated with Microbial Presence Microbial Absence

Castile Brine 169 x 10-7 M 177 x 10-7 MSalado Formation Brine 307 x 10-7 M 307 x 10-7 M

Brush LH and Xiong Y Actinide Solubility for the WIPP PAB Calculations unpublished analysis (2005)


DOE weapons complex The WIPP is located in southeastern New Mexico 26 miles east of Carlsbad Waste disposal operations began on March 26 1999

The Waste Isolation Pilot Plant WIPP a cornerstone of the DOE s cleanup effort is designed to permanently dispose of defense-generated transuranic radioactive waste from research and production activities in the



















Lab Capability





speciation

















NaCl simplified


MgCl26H2O 3667 0018 1934 0953 7519 3704

Na2SO4 2252 0159 2361 0166

NaBr 1074 0010 2565 0025Na2B4O710H2O 57 0015 1403 0037

KCl 6869 0092 3257 0437

LiCl - - 0174 0004

CaCl22H2O 1672 0011 1896 0013





0 20 40 60 80 100 120 140 160 18000

01

02

03

04

05

06

07

08

09

Abs

orba

nce

at 3

51 n

m

Time hours

GWB at pcH = 85 y = 0836e-0012t

ERDA-6 at pcH = 90 y = 0789e-0075t


250 275 300 325 350 375 400

000

002

004

006

008

010

012

014

016

Abs

orba

nce

(rel

uni

t)Wavelength (nm)


OCl- in 5 M NaCl

2 OCl- + H2O2 2 Cl- + H2O + O2




0 100 200 300 400 500 6000000

0001

0002

0003

0004

0005

0006

5 m NaCl

4 m NaCl

3 m NaCl

2 m NaCl

H

ypoc

hlor

ite C

once

ntra

tion

M

Dose (kGy)



0 1 2 3 4 5 6 7 8 9 10 11 12 13000

001

002

003

004

005

006

Hyp

ochl

orite

Sat

urat

ion

M

238Pu Activity CiL

5 M NaCl

0380402044032305002740550235

GClOHGH2O2

Cl-concentration

[M]




0 100 200 300 400 500 600

0

1x10-5

2x10-5

3x10-5

4x10-5

5x10-5

Pu

conc

entra

tion

MTime in hours

Ferric oxide

Fe Powder

Fe Coupon

Magnetite





300 400 500 600 700 800 900

000

002

004

006

008

010

Opt

ical

Den

sity

Wavelength (nm)

Pu(VI) in GWB Brine












00 05 10 15 20 250

2

4

6

8

10

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09998 pcH - 09438




00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)



























Lab Capability





speciation

















NaCl simplified


MgCl26H2O 3667 0018 1934 0953 7519 3704

Na2SO4 2252 0159 2361 0166

NaBr 1074 0010 2565 0025Na2B4O710H2O 57 0015 1403 0037

KCl 6869 0092 3257 0437

LiCl - - 0174 0004

CaCl22H2O 1672 0011 1896 0013





0 20 40 60 80 100 120 140 160 18000

01

02

03

04

05

06

07

08

09

Abs

orba

nce

at 3

51 n

m

Time hours

GWB at pcH = 85 y = 0836e-0012t

ERDA-6 at pcH = 90 y = 0789e-0075t


250 275 300 325 350 375 400

000

002

004

006

008

010

012

014

016

Abs

orba

nce

(rel

uni

t)Wavelength (nm)


OCl- in 5 M NaCl

2 OCl- + H2O2 2 Cl- + H2O + O2




0 100 200 300 400 500 6000000

0001

0002

0003

0004

0005

0006

5 m NaCl

4 m NaCl

3 m NaCl

2 m NaCl

H

ypoc

hlor

ite C

once

ntra

tion

M

Dose (kGy)



0 1 2 3 4 5 6 7 8 9 10 11 12 13000

001

002

003

004

005

006

Hyp

ochl

orite

Sat

urat

ion

M

238Pu Activity CiL

5 M NaCl

0380402044032305002740550235

GClOHGH2O2

Cl-concentration

[M]




0 100 200 300 400 500 600

0

1x10-5

2x10-5

3x10-5

4x10-5

5x10-5

Pu

conc

entra

tion

MTime in hours

Ferric oxide

Fe Powder

Fe Coupon

Magnetite





300 400 500 600 700 800 900

000

002

004

006

008

010

Opt

ical

Den

sity

Wavelength (nm)

Pu(VI) in GWB Brine












00 05 10 15 20 250

2

4

6

8

10

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09998 pcH - 09438




00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)












speciation

















NaCl simplified


MgCl26H2O 3667 0018 1934 0953 7519 3704

Na2SO4 2252 0159 2361 0166

NaBr 1074 0010 2565 0025Na2B4O710H2O 57 0015 1403 0037

KCl 6869 0092 3257 0437

LiCl - - 0174 0004

CaCl22H2O 1672 0011 1896 0013





0 20 40 60 80 100 120 140 160 18000

01

02

03

04

05

06

07

08

09

Abs

orba

nce

at 3

51 n

m

Time hours

GWB at pcH = 85 y = 0836e-0012t

ERDA-6 at pcH = 90 y = 0789e-0075t


250 275 300 325 350 375 400

000

002

004

006

008

010

012

014

016

Abs

orba

nce

(rel

uni

t)Wavelength (nm)


OCl- in 5 M NaCl

2 OCl- + H2O2 2 Cl- + H2O + O2




0 100 200 300 400 500 6000000

0001

0002

0003

0004

0005

0006

5 m NaCl

4 m NaCl

3 m NaCl

2 m NaCl

H

ypoc

hlor

ite C

once

ntra

tion

M

Dose (kGy)



0 1 2 3 4 5 6 7 8 9 10 11 12 13000

001

002

003

004

005

006

Hyp

ochl

orite

Sat

urat

ion

M

238Pu Activity CiL

5 M NaCl

0380402044032305002740550235

GClOHGH2O2

Cl-concentration

[M]




0 100 200 300 400 500 600

0

1x10-5

2x10-5

3x10-5

4x10-5

5x10-5

Pu

conc

entra

tion

MTime in hours

Ferric oxide

Fe Powder

Fe Coupon

Magnetite





300 400 500 600 700 800 900

000

002

004

006

008

010

Opt

ical

Den

sity

Wavelength (nm)

Pu(VI) in GWB Brine












00 05 10 15 20 250

2

4

6

8

10

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09998 pcH - 09438




00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)























NaCl simplified


MgCl26H2O 3667 0018 1934 0953 7519 3704

Na2SO4 2252 0159 2361 0166

NaBr 1074 0010 2565 0025Na2B4O710H2O 57 0015 1403 0037

KCl 6869 0092 3257 0437

LiCl - - 0174 0004

CaCl22H2O 1672 0011 1896 0013





0 20 40 60 80 100 120 140 160 18000

01

02

03

04

05

06

07

08

09

Abs

orba

nce

at 3

51 n

m

Time hours

GWB at pcH = 85 y = 0836e-0012t

ERDA-6 at pcH = 90 y = 0789e-0075t


250 275 300 325 350 375 400

000

002

004

006

008

010

012

014

016

Abs

orba

nce

(rel

uni

t)Wavelength (nm)


OCl- in 5 M NaCl

2 OCl- + H2O2 2 Cl- + H2O + O2




0 100 200 300 400 500 6000000

0001

0002

0003

0004

0005

0006

5 m NaCl

4 m NaCl

3 m NaCl

2 m NaCl

H

ypoc

hlor

ite C

once

ntra

tion

M

Dose (kGy)



0 1 2 3 4 5 6 7 8 9 10 11 12 13000

001

002

003

004

005

006

Hyp

ochl

orite

Sat

urat

ion

M

238Pu Activity CiL

5 M NaCl

0380402044032305002740550235

GClOHGH2O2

Cl-concentration

[M]




0 100 200 300 400 500 600

0

1x10-5

2x10-5

3x10-5

4x10-5

5x10-5

Pu

conc

entra

tion

MTime in hours

Ferric oxide

Fe Powder

Fe Coupon

Magnetite





300 400 500 600 700 800 900

000

002

004

006

008

010

Opt

ical

Den

sity

Wavelength (nm)

Pu(VI) in GWB Brine












00 05 10 15 20 250

2

4

6

8

10

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09998 pcH - 09438




00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)











0 20 40 60 80 100 120 140 160 18000

01

02

03

04

05

06

07

08

09

Abs

orba

nce

at 3

51 n

m

Time hours

GWB at pcH = 85 y = 0836e-0012t

ERDA-6 at pcH = 90 y = 0789e-0075t


250 275 300 325 350 375 400

000

002

004

006

008

010

012

014

016

Abs

orba

nce

(rel

uni

t)Wavelength (nm)


OCl- in 5 M NaCl

2 OCl- + H2O2 2 Cl- + H2O + O2




0 100 200 300 400 500 6000000

0001

0002

0003

0004

0005

0006

5 m NaCl

4 m NaCl

3 m NaCl

2 m NaCl

H

ypoc

hlor

ite C

once

ntra

tion

M

Dose (kGy)



0 1 2 3 4 5 6 7 8 9 10 11 12 13000

001

002

003

004

005

006

Hyp

ochl

orite

Sat

urat

ion

M

238Pu Activity CiL

5 M NaCl

0380402044032305002740550235

GClOHGH2O2

Cl-concentration

[M]




0 100 200 300 400 500 600

0

1x10-5

2x10-5

3x10-5

4x10-5

5x10-5

Pu

conc

entra

tion

MTime in hours

Ferric oxide

Fe Powder

Fe Coupon

Magnetite





300 400 500 600 700 800 900

000

002

004

006

008

010

Opt

ical

Den

sity

Wavelength (nm)

Pu(VI) in GWB Brine












00 05 10 15 20 250

2

4

6

8

10

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09998 pcH - 09438




00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)











0 100 200 300 400 500 6000000

0001

0002

0003

0004

0005

0006

5 m NaCl

4 m NaCl

3 m NaCl

2 m NaCl

H

ypoc

hlor

ite C

once

ntra

tion

M

Dose (kGy)



0 1 2 3 4 5 6 7 8 9 10 11 12 13000

001

002

003

004

005

006

Hyp

ochl

orite

Sat

urat

ion

M

238Pu Activity CiL

5 M NaCl

0380402044032305002740550235

GClOHGH2O2

Cl-concentration

[M]




0 100 200 300 400 500 600

0

1x10-5

2x10-5

3x10-5

4x10-5

5x10-5

Pu

conc

entra

tion

MTime in hours

Ferric oxide

Fe Powder

Fe Coupon

Magnetite





300 400 500 600 700 800 900

000

002

004

006

008

010

Opt

ical

Den

sity

Wavelength (nm)

Pu(VI) in GWB Brine












00 05 10 15 20 250

2

4

6

8

10

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09998 pcH - 09438




00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)











0 1 2 3 4 5 6 7 8 9 10 11 12 13000

001

002

003

004

005

006

Hyp

ochl

orite

Sat

urat

ion

M

238Pu Activity CiL

5 M NaCl

0380402044032305002740550235

GClOHGH2O2

Cl-concentration

[M]




0 100 200 300 400 500 600

0

1x10-5

2x10-5

3x10-5

4x10-5

5x10-5

Pu

conc

entra

tion

MTime in hours

Ferric oxide

Fe Powder

Fe Coupon

Magnetite





300 400 500 600 700 800 900

000

002

004

006

008

010

Opt

ical

Den

sity

Wavelength (nm)

Pu(VI) in GWB Brine












00 05 10 15 20 250

2

4

6

8

10

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09998 pcH - 09438




00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)











0 100 200 300 400 500 600

0

1x10-5

2x10-5

3x10-5

4x10-5

5x10-5

Pu

conc

entra

tion

MTime in hours

Ferric oxide

Fe Powder

Fe Coupon

Magnetite





300 400 500 600 700 800 900

000

002

004

006

008

010

Opt

ical

Den

sity

Wavelength (nm)

Pu(VI) in GWB Brine












00 05 10 15 20 250

2

4

6

8

10

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09998 pcH - 09438




00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)











300 400 500 600 700 800 900

000

002

004

006

008

010

Opt

ical

Den

sity

Wavelength (nm)

Pu(VI) in GWB Brine












00 05 10 15 20 250

2

4

6

8

10

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09998 pcH - 09438




00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)



















00 05 10 15 20 250

2

4

6

8

10

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09998 pcH - 09438




00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)











00 05 10 15 20 25 30 35 40 45 500

2

4

6

8

0 2 40

2

4

pH re

adin

g



Buffering by borate


pH re

adin

g

pCH+ calculated


pHread = 09749 pcH - 1229


ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










ERDA-6







ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










ERDA-6 cont





0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










0 2 4 6 8 10 12 14 16 18 20 22 2410-8

10-7

10-6

10-5

10-4

pCH+

- 80 - 90 - 92

N

d C

once

ntra

tion

M



oversaturation

Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4


Nd

Con

cent

ratio

n M

pCH+



Nd (III)


70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










70 75 80 85 90 95 100 105 1101E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+


- trend (no carb)


with carbonates

Nd (III)


0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










0 25 50 75 100 125 15010-10

10-9

10-8

10-7

10-6

10-5

10-4

10-3

10-2


Ura

nium

con

cent

ratio

n M

Time Days



U (VI)


8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










8 9 10 11 1210-10

10-9

10-8

10-7

10-6

10-5

ERDA-6


Ura

nium

con

cent

ratio

n M

pCH+



U (VI)








GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)
















GWB CONT





60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



with carbonates

Nd (III)


60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










60 65 70 75 80 85 901E-9

1E-8

1E-7

1E-6

1E-5

1E-4

N

d C

once

ntra

tion

M

pCH+



carbonate free

Nd (III)


0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










0 25 50 75 100 125 15010-7

10-6

10-5

10-4

10-3

Ura

nium

con

cent

ratio

n M

Time Days


GWB carbonate free

U (VI)


U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










U (VI)

60 65 70 75 80 85 901E-7

1E-6

1E-5

1E-4

Ura

nium

con

cent

ratio

n M

pCH+



5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










5 M NaCl







70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)










70 75 80 85 90 95 100 105 110 115 120 125 1301E-9

1E-8

1E-7

1E-6

1E-5

1E-4

Nd

Con

cent

ratio

n M

pCH+



carbonate free

Nd (III)









actinide chemistry and repository science program in ......ans 14th biennial topical meeting la-ur...

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