electronic supplementary information revised s1-s17 · cameron c. ellis, nishat tasnim, supriyo...

32
Electronic Supplementary Information Synthesis and Characterization of a Photocleavable Collagen-Like Peptide Alfredo Ornelas, Kaitlyn N. Williams, Kevin A. Hatch, Aurelio Paez, Angela C. Aguilar, Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael* Table of content Collagen-like peptide 1 HR ESI-TOF-MS ………………………………………………………………… S3 Comparison of actual MS and isotopic simulation …………………………….. S4 FPLC profile ……………………………………………………………………… S5 Amino acid building block 6 HR ESI-TOF-MS ………………………………………………………………… S6 1 H NMR spectrum ……………………………………………………………….. S7 13 NMR spectrum …………………………………………………………………. S8 Peptide building block 7 HR ESI-TOF-MS …………………………………………………………………. S9 Comparison of actual MS and isotopic simulation …………………………….. S10 FPLC profile ……………………………………………………………………… S11 N-Fmoc-glycyl-5-bromo-7-nitroindoline (13) HR ESI-TOF-MS …………………………………………………………………. S12 1 H NMR spectrum ………………………………………………………………… S13 13 NMR spectrum ………………………………………………………………….. S14 Allyl N-(Fmoc-glycyl)-5-carboxylate-7-nitroindoline (16) HR ESI-TOF-MS …………………………………………………………………. S15 1 H NMR spectrum ………………………………………………………………… S16 13 NMR spectrum ………………………………………………………………….. S17 S1 Electronic Supplementary Material (ESI) for Organic & Biomolecular Chemistry. This journal is © The Royal Society of Chemistry 2018

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Page 1: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

ElectronicSupplementaryInformation

Synthesis and Characterization of a Photocleavable Collagen-Like Peptide Alfredo Ornelas, Kaitlyn N. Williams, Kevin A. Hatch, Aurelio Paez, Angela C. Aguilar, Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael* Table of content Collagen-like peptide 1 HR ESI-TOF-MS ………………………………………………………………… S3 Comparison of actual MS and isotopic simulation …………………………….. S4 FPLC profile ……………………………………………………………………… S5 Amino acid building block 6 HR ESI-TOF-MS ………………………………………………………………… S6 1H NMR spectrum ……………………………………………………………….. S7 13NMR spectrum …………………………………………………………………. S8 Peptide building block 7 HR ESI-TOF-MS …………………………………………………………………. S9 Comparison of actual MS and isotopic simulation …………………………….. S10 FPLC profile ……………………………………………………………………… S11 N-Fmoc-glycyl-5-bromo-7-nitroindoline (13) HR ESI-TOF-MS …………………………………………………………………. S12 1H NMR spectrum ………………………………………………………………… S13 13NMR spectrum ………………………………………………………………….. S14 Allyl N-(Fmoc-glycyl)-5-carboxylate-7-nitroindoline (16) HR ESI-TOF-MS …………………………………………………………………. S15 1H NMR spectrum ………………………………………………………………… S16 13NMR spectrum ………………………………………………………………….. S17

S1

Electronic Supplementary Material (ESI) for Organic & Biomolecular Chemistry.This journal is © The Royal Society of Chemistry 2018

Page 2: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Liquid Chromatography-Mass Spectrometry (LC-MS) and MS/MS analysis of the photodecomposition products of peptide 1 obtained upon illumination with UV light at 350 nm in water TotalIonCount(TIC)chromatogramofthephotodecomositionproducts ofpeptide1.................................................................................................................................... S18 MSofpeptide9elutingat40.94min…………………………………………………………….S19 MSofpeptide9elutingat41.38min…………………………………………………………….S20 MSofpeptide17elutingat41.92min………………………………………………………….S21 MSofpeptides9and17elutingat41.96min……………………………………………….S22 MSofpeptide18elutingat45.47min………………………………………………………... S23 MS/MSofpeptide18…………………………………………………………………………………. S24 MSofpeptide19elutingat45.89min………………………………………………………... S25 MS/MSofpeptide19…………………………………………………………………………………. S26 MSofpeptide11elutingat50.98min………………………………………………………... S27 MSofpeptides10and12elutingat51.37min…………………………………………….S28 MSofpeptides10and12elutingat51.47min…………………………………………….S29 MSofpeptide17elutingat51.76min………………………………………………………….S30 MSofpeptide20elutingat52.13min………………………………………………………….S31 MS/MSofpeptide20…………………………………………………………………………………. S32

S2

Page 3: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

HRESITOFMSofpeptide1. m/z [M+2H]2+ calcd. 1685.7205 (most abundant species), obs. 1685.7175; [M+3H]3+ calcd. 1123.8153 (monoisotopic species), obs. 1123.8211.

S3

H-Pro-Pro-Gly-Hyp-Pro-Gly-Ind-Pro-Pro-Gly-Hyp-Pro-Gly-Ind-Pro-Pro-Gly-Hyp-Pro-Gly-Ind-Pro-Pro-Gly-Hyp-Pro-Gly-Ind-Pro-Pro-Gly-Hyp-Pro-Gly-NH2

N

O2NHN

ON

ON

HO

ONH

ON

ONO

O HN

ON

ON

HO

ONH

ON

ON

ON

O2NHN

ON

ON

HO

ONH

ON

ON

O

5-carboxy-7-nitroindolinylmoiety

5-carboxy-7-nitroindolinylmoiety

O

1

Page 4: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Actual (top) and simulated mass spectrum (bottom) of peptide 1 m/z [M+2H]2+ (most abundant peak) calcd. 1685.7205, obs. 1685.7175.

Actual (top) and simulated mass spectrum (bottom) of peptide 1 (m/z)[M+3H]3+ calcd. 1123.8061 (monoisotopic species), obs. 1123.8211.

S4

Page 5: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

ReversedPhaseFPLCprofileofpeptide1.Stationaryphase:15 µm diameter polystyrene/divinyl benzene beads; Solvent A: 2% CH3CN and 0.1% TFA in water, solvent B: 85% CH3CN and0.1%TFAinwater;Gradient(green):0-90%B.Detectionat250nm(blue),350nm(red),and430nm(pink).

S5

H-Pro-Pro-Gly-Hyp-Pro-Gly-Ind-Pro-Pro-Gly-Hyp-Pro-Gly-Ind-Pro-Pro-Gly-Hyp-Pro-Gly-Ind-Pro-Pro-Gly-Hyp-Pro-Gly-Ind-Pro-Pro-Gly-Hyp-Pro-Gly-NH2

N

O2NHN

ON

ON

HO

ONH

ON

ONO

O HN

ON

ON

HO

ONH

ON

ON

ON

O2NHN

ON

ON

HO

ONH

ON

ON

O

5-carboxy-7-nitroindolinylmoiety

5-carboxy-7-nitroindolinylmoiety

O

1

Page 6: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

HR ESI TOF MS of amino acid building block 6, m/z [M-H]- calcd. 486.1301; obs. 486.1327.

S6

NNO2

HOOC

O

NHFmoc6

Page 7: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

1HNMRspectrumofcompound6.

S7

NNO2

HOOC

O

NHFmoc6

Page 8: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

13CNMRspectrumofcompound6.

S8

NNO2

HOOC

O

NHFmoc6

Page 9: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

HRESITOFMSofpeptide7,m/z [M+H]+ calcd.: 1005.4358; obs. 1005.4334; [M+Na]+ calcd. 1027.4178; obs. 1027.4150.

S9

GlyProHypGlyProProFmoctBu

7

COOH

NNO2

Page 10: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Actual (top) and simulated mass spectrum (bottom) of peptide 7, m/z [M+H]+ calcd.: 1005.4358; obs. 1005.4334.

S10

Page 11: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

ReversedPhaseFPLCprofileofpeptide7.Stationaryphase:15 µm diameter polystyrene/divinyl benzene beads; Solvent A: 2% CH3CN and 0.1% TFA in water, solvent B: 85% CH3CN and0.1%TFAinwater;Gradient(green):0-90%B.Detectionat250nm(blue),350nm(red),and430nm(pink).

S11

GlyProHypGlyProProFmoctBu

7

COOH

NNO2

Page 12: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

HR ESI TOF MS of compound 13; m/z [M+NH4]+ calcd. 539.0930 and 541.0913, obs. 539.0904 and 541.0937; [M+Na]+ calcd. 544.0484 and 546.0467, obs. 544.0489 and 546.0463.

S12

NNO2

Br

O

NHFmoc13

Page 13: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

1H NMR spectrum of compound 13.

S13

NNO2

Br

O

NHFmoc13

Page 14: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

13CNMRspectrumofcompound13.

S14

NNO2

Br

O

NHFmoc13

Page 15: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

HR-ESI-TOF-MS of compound 16; m/z [M+Na]+ calcd. 550.1590, obs. 550.1597; [M+K]+ calcd. 566.1330, obs. 566.1333.

S15

N

AllOOC

NO2

16

O

NHFmoc

Page 16: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

1HNMRspectrumofcompound16.

S16

N

AllOOC

NO2

16

O

NHFmoc

Page 17: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

13CNMRspectrumofcompound16.

S17

N

AllOOC

NO2

16

O

NHFmoc

Page 18: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 0.00 - 60.00 SM: 3B

0 5 10 15 20 25 30 35 40 45 50 55 60Time (min)

0

5

10

15

20

25

30

35

40

45

50

55

60

65

70

75

80

85

90

95

100

Re

lative

Ab

un

da

nce

40.98

41.33

45.8442.30

51.5142.97 51.59

51.8153.1151.04

45.48

47.71

49.28

40.3856.08

8.598.31 33.10 56.419.166.58 34.06 37.584.85 27.7426.78 28.8719.793.12 24.1117.9715.9513.87

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

Total Ion Count (TIC)-based Nano-UHPLC chromatogram of the peptide fragments obtained after irradiation of the full length peptide 1 with 350 nm light in water.

S18

Page 19: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Top: TIC chromatogram of photolysis products of peptide 1, irradiated with near UV light (350 nm) in water. Bottom: HRMS of peptide 9 eluting at 40.94 min: m/z [M+H]

+ calcd. 537.2673, obs. 537.2678.

S19

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 35.00 - 60.00 SM: 3B

35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60Time (min)

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

40.9840.91

41.07

41.11

41.22

41.3345.8442.30

51.5142.3941.4651.81 53.1143.07 51.04

45.4843.1447.7147.3843.91 44.26 49.28 49.6648.7640.38 46.3840.18 56.0853.68 56.4154.12 55.72 59.9858.3139.3837.5837.1736.39

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

CLP_Irradiated_Alfredo_DrMichael_171208195110 #12892 RT: 40.94 AV: 1 NL: 1.49E10T: FTMS + p NSI Full ms [300.0000-1600.0000]

300 400 500 600 700 800 900 1000 1100 1200 1300 1400 1500 1600m/z

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

537.2678

Page 20: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Top: TIC chromatogram of photolysis products of peptide 1, irradiated with near UV light (350 nm) in water. Bottom: HRMS of peptide 9 eluting at 41.38 min: m/z [M+H]

+ calcd. 537.2673, obs. 537.2676.

S20

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 35.00 - 60.00 SM: 3B

35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60Time (min)

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

40.9840.91

41.07

41.11

41.22

41.3345.8442.30

51.5142.3941.4651.81 53.1143.07 51.04

45.4843.1447.7147.3843.91 44.26 49.28 49.6648.7640.38 46.3840.18 56.0853.68 56.4154.12 55.72 59.9858.3139.3837.5837.1736.39

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

CLP_Irradiated_Alfredo_DrMichael_171208195110 #13013 RT: 41.38 AV: 1 NL: 3.92E9T: FTMS + p NSI Full lock ms [300.0000-1600.0000]

300 400 500 600 700 800 900 1000 1100 1200 1300 1400 1500 1600m/z

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

537.2676

Page 21: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Top: TIC chromatogram of photolysis products of peptide 1, irradiated with near UV light (350 nm) in water. Bottom: HRMS of peptide 17 eluting at 41.92 min: m/z [M+NH4]

+ calcd. 744.3317, obs.

744.3313; m/z [M+H+NH4]2+

calcd. 372.6697, obs. 372.6693.

S21

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 35.00 - 60.00 SM: 3B

35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60Time (min)

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

40.9840.91

41.07

41.11

41.22

41.3345.8442.30

51.5142.3941.4651.81 53.1143.07 51.04

45.4843.1447.7147.3843.91 44.26 49.28 49.6648.7640.38 46.3840.18 56.0853.68 56.4154.12 55.72 59.9858.3139.3837.5837.1736.39

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

CLP_Irradiated_Alfredo_DrMichael_171208195110 #13248 RT: 41.92 AV: 1 NL: 6.23E8T: FTMS + p NSI Full lock ms [300.0000-1600.0000]

300 400 500 600 700 800 900 1000 1100 1200 1300 1400 1500 1600m/z

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

762.3417

372.6693

744.3313381.6744

780.3522535.2512 705.3204344.1585 391.6424

Peptide 17

unidentified

Page 22: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Top: TIC chromatogram of photolysis products of peptide 1, irradiated with near UV light (350 nm) in water. Bottom: HRMS of peptides 9 and 17 eluting at 41.96 min: 9, m/z [M+H]

+ calcd. 537.2673, obs.

537.2663; 17, m/z [M+NH4]+ calcd. 744.3317, obs. 744.3303; m/z [M+H+NH4]

2+ calcd.

372.6697, obs. 372.6690.

S22

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 35.00 - 60.00 SM: 3B

35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60Time (min)

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

40.9840.91

41.07

41.11

41.22

41.3345.8442.30

51.5142.3941.4651.81 53.1143.07 51.04

45.4843.1447.7147.3843.91 44.26 49.28 49.6648.7640.38 46.3840.18 56.0853.68 56.4154.12 55.72 59.9858.3139.3837.5837.1736.39

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

CLP_Irradiated_Alfredo_DrMichael_171208195110 #13263 RT: 41.96 AV: 1 NL: 7.03E8T: FTMS + p NSI Full lock ms [300.0000-1600.0000]

300 400 500 600 700 800 900 1000 1100 1200 1300 1400 1500 1600m/z

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

372.6690z=2

762.3408z=2537.2663

z=1

381.6738z=2

744.3303z=1

780.3510z=?

569.2560z=1

391.6419z=2

705.3196z=1

344.1581z=2

Peptide 9

Peptide 17

Page 23: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Top: TIC chromatogram of photolysis products of peptide 1, irradiated with near UV light (350 nm) in water. Bottom: HRMS of peptide 18 eluting at 45.47 min: m/z [M+H]+ calcd. 710.3262, obs. 710.3259; m/z [M+2H]2+ calcd. 355.6670, obs. 355.6664.

S23

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 35.00 - 60.00 SM: 3B

35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60Time (min)

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

40.9840.91

41.07

41.11

41.22

41.3345.8442.30

51.5142.3941.4651.81 53.1143.07 51.04

45.4843.1447.7147.3843.91 44.26 49.28 49.6648.7640.38 46.3840.18 56.0853.68 56.4154.12 55.72 59.9858.3139.3837.5837.1736.39

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

CLP_Irradiated_Alfredo_DrMichael_171208195110 #14889 RT: 45.47 AV: 1 NL: 1.91E9T: FTMS + p NSI Full lock ms [300.0000-1600.0000]

300 400 500 600 700 800 900 1000 1100 1200 1300 1400 1500 1600m/z

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

710.3259z=2

355.6664z=2

579.2774z=1

Page 24: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

MS/MS spectrum of peptide 18: N-terminal nitrosoindoline fragment, C9H7N2O2, m/z [M]+

calcd. 175.0508, obs. 175.0501; protonated C-terminal fragment, C24H38N7O7, m/z [M+H]+ calcd. 536.2833, obs. 536.2835.

S24

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

CLP_Irradiated_Alfredo_DrMichael_171208195110 #14566-16057 RT: 45.31-47.11 AV: 2 RF: 6.00,3 NL: 1.75E7F: FTMS + c NSI d Full ms2 710.3259

100 200 300 400 500 600 700 800 900 1000 1100 1200 1300 1400m/z

0

5

10

15

20

25

30

35

40

45

50

55

60

65

70

75

80

85

90

95

100

Rel

ativ

e A

bund

ance

175.0501z=1

536.2825z=1

272.1025z=1

286.1380z=?

244.1077z=1

439.2294z=1

159.0552z=? 342.1774

z=? 519.2554z=?

559.2510z=1

98.0604z=? 710.2731

z=1866.3157

z=11117.4409

z=?

N

NN

NO

O

NHO

HO

O O

O

NH2

HN

O

NH

NO

18

Page 25: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Top: TIC chromatogram of photolysis products of peptide 1, irradiated with near UV light (350 nm) in water. Bottom: HRMS of peptide 19 eluting at 45.89 min: m/z [M+H]+ calcd. 711.3102, obs. 711.3093; m/z [M+H]2+ calcd. 356.1590, obs. 356.1580.

S25

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 35.00 - 60.00 SM: 3B

35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60Time (min)

0

10

20

30

40

50

60

70

80

90

100

Re

lativ

e A

bu

nd

an

ce

40.9840.91

41.07

41.11

41.22

41.3345.8442.30

51.5142.3941.4651.81 53.1143.07 51.04

45.4843.1447.7147.3843.91 44.26 49.28 49.6648.7640.38 46.3840.18 56.0853.68 56.4154.12 55.72 59.9858.3139.3837.5837.1736.39

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

CLP_Irradiated_Alfredo_DrMichael_171208195110 #15087 RT: 45.89 AV: 1 NL: 2.82E9T: FTMS + p NSI Full ms [300.0000-1600.0000]

300 400 500 600 700 800 900 1000 1100 1200 1300 1400 1500 1600m/z

0

10

20

30

40

50

60

70

80

90

100

Re

lativ

e A

bu

nd

an

ce

711.3093z=2

356.1580z=2

Page 26: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

MS/MS spectrum of peptide 19: N-terminal nitrosoindoline fragment, C9H7N2O2, m/z [M]+

calcd. 175.0508, obs. 175.0501; protonated C-terminal fragment, C24H37N6O8, m/z [M+H]+ calcd. 537.2673, obs. 537.2672.

S26

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

CLP_Irradiated_Alfredo_DrMichael_171208195110 #14559-16129 RT: 45.67-46.60 AV: 3 RF: 6.00,3 NL: 2.51E7F: FTMS + c NSI d Full ms2 711.3093

100 200 300 400 500 600 700 800 900 1000 1100 1200 1300 1400m/z

0

5

10

15

20

25

30

35

40

45

50

55

60

65

70

75

80

85

90

95

100

Rel

ativ

e A

bund

ance

175.0501z=1

272.1025z=1 537.2672

z=1

244.1077z=1

440.2130z=1

343.1603z=?

155.0813z=?

519.2557z=?

713.2845z=2

598.2021z=?

851.3367z=?

1102.4276z=?

1036.3981z=?

N

NN

NO

O

NHO

HO

O O

O

OH

HN

O

NH

NO

19

Page 27: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Top: TIC chromatogram of photolysis products of peptide 1, irradiated with near UV light (350 nm) in water. Bottom: HRMS of peptide 11 eluting at 50.98 min: m/z [M+H]+ calcd. 708.3105, obs. 708.3095.

S27

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 35.00 - 60.00 SM: 3B

35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60Time (min)

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

40.9840.91

41.07

41.11

41.22

41.3345.8442.30

51.5142.3941.4651.81 53.1143.07 51.04

45.4843.1447.7147.3843.91 44.26 49.28 49.6648.7640.38 46.3840.18 56.0853.68 56.4154.12 55.72 59.9858.3139.3837.5837.1736.39

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

CLP_Irradiated_Alfredo_DrMichael_171208195110 #17473 RT: 50.98 AV: 1 NL: 2.56E9T: FTMS + p NSI Full ms [300.0000-1600.0000]

675 680 685 690 695 700 705 710 715 720 725 730 735 740 745 750 755 760 765m/z

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

708.3095z=1

709.3121z=1

Page 28: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Top: TIC chromatogram of photolysis products of peptide 1, irradiated with near UV light (350 nm) in water. Bottom: HRMS of peptides 10 and 12 eluting at 51.37 min: 10, m/z [M+H]+ calcd. 709.2946, obs. 709.2946; 12, m/z [M+H]+ calcd. 726.3211, obs. 726.3209.

S28

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 35.00 - 60.00 SM: 3B

35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60Time (min)

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

40.9840.91

41.07

41.11

41.22

41.3345.8442.30

51.5142.3941.4651.81 53.1143.07 51.04

45.4843.1447.7147.3843.91 44.26 49.28 49.6648.7640.38 46.3840.18 56.0853.68 56.4154.12 55.72 59.9858.3139.3837.5837.1736.39

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

CLP_Irradiated_Alfredo_DrMichael_171208195110 #17665 RT: 51.37 AV: 1 NL: 1.30E9T: FTMS + p NSI Full lock ms [300.0000-1600.0000]

300 400 500 600 700 800 900 1000 1100 1200 1300 1400 1500 1600m/z

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

726.3209z=1

709.2946z=1

Peptide 10

Peptide 12

Page 29: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Top: TIC chromatogram of photolysis products of peptide 1, irradiated with near UV light (350 nm) in water. Bottom: HRMS of peptides 10 and 12 eluting at 51.47 min: 10, m/z [M+H]+ calcd. 709.2946, obs. 709.2943; 12, m/z [M+H]+ calcd. 726.3211, obs. 726.3203.

S29

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 35.00 - 60.00 SM: 3B

35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60Time (min)

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

40.9840.91

41.07

41.11

41.22

41.3345.8442.30

51.5142.3941.4651.81 53.1143.07 51.04

45.4843.1447.7147.3843.91 44.26 49.28 49.6648.7640.38 46.3840.18 56.0853.68 56.4154.12 55.72 59.9858.3139.3837.5837.1736.39

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

CLP_Irradiated_Alfredo_DrMichael_171208195110 #17711 RT: 51.47 AV: 1 NL: 2.45E9T: FTMS + p NSI Full ms [300.0000-1600.0000]

350 400 450 500 550 600 650 700 750 800 850 900 950 1000 1050 1100 1150 1200 1250 1300 1350 1400m/z

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

709.2943z=1

726.3203z=1

Peptide 10

Peptide 12

Page 30: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Top: TIC chromatogram of photolysis products of peptide 1, irradiated with near UV light (350 nm) in water. Bottom: HRMS of peptide 17 eluting at 51.76 min: m/z [M+H]+ calcd. 727.3051, obs. 727.3049; m/z [M+NH4]+ calcd. 744.3317, obs. 744.3312.

S30

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 35.00 - 60.00 SM: 3B

35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60Time (min)

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

40.9840.91

41.07

41.11

41.22

41.3345.8442.30

51.5142.3941.4651.81 53.1143.07 51.04

45.4843.1447.7147.3843.91 44.26 49.28 49.6648.7640.38 46.3840.18 56.0853.68 56.4154.12 55.72 59.9858.3139.3837.5837.1736.39

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

CLP_Irradiated_Alfredo_DrMichael_171208195110 #17827 RT: 51.76 AV: 1 NL: 1.92E9T: FTMS + p NSI Full ms [300.0000-1600.0000]

350 400 450 500 550 600 650 700 750 800 850 900 950 1000 1050 1100 1150 1200 1250 1300 1350 1400m/z

0

10

20

30

40

50

60

70

80

90

100

Re

lative

Ab

un

da

nce

727.3049z=1

744.3312z=?

Page 31: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

Top: TIC chromatogram of photolysis products of peptide 1, irradiated with near UV light (350 nm) in water. Bottom: HRMS of peptide 20 eluting at 52.13 min: m/z [M+H]+ calcd. 725.2895, obs. 725.2885; m/z [M+NH4]+ calcd. 742.3160, obs. 742.3148.

S31

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

RT: 35.00 - 60.00 SM: 3B

35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60Time (min)

0

10

20

30

40

50

60

70

80

90

100

Re

lativ

e A

bu

nd

an

ce

40.9840.91

41.07

41.11

41.22

41.3345.8442.30

51.5142.3941.4651.81 53.1143.07 51.04

45.4843.1447.7147.3843.91 44.26 49.28 49.6648.7640.38 46.3840.18 56.0853.68 56.4154.12 55.72 59.9858.3139.3837.5837.1736.39

NL: 2.78E10TIC F: FTMS + p NSI Full ms [300.0000-1600.0000] MS CLP_Irradiated_Alfredo_DrMichael_171208195110

CLP_Irradiated_Alfredo_DrMichael_171208195110 #17996 RT: 52.13 AV: 1 NL: 8.76E8T: FTMS + p NSI Full lock ms [300.0000-1600.0000]

400 450 500 550 600 650 700 750 800 850 900 950 1000 1050 1100 1150 1200 1250 1300 1350 1400 1450m/z

0

10

20

30

40

50

60

70

80

90

100

Re

lativ

e A

bu

nd

an

ce

725.2885z=1

742.3148z=1

Page 32: Electronic Supplementary Information revised S1-S17 · Cameron C. Ellis, Nishat Tasnim, Supriyo Ray, Carl W. Dirk, Thomas Boland, Binata Joddar, Chunqiang Li,* and Katja Michael*

MS/MS spectrum of peptide 20: N-terminal nitroindole fragment, C9H5N2O3, m/z [M]+ calcd. 189.0300 , obs. 189.0293; protonated C-terminal tripeptide fragment, C12H20N3O5, m/z [M+H]+

calcd. 286.1403, obs. 286.1391.

S32

CLP_Irradiated_Alfredo_DrMichael_1712... 12/08/17 19:55:45

CLP_Irradiated_Alfredo_DrMichael_171208195110 #17670-18477 RT: 51.96-52.75 AV: 3 RF: 6.00,3 NL: 9.50E7F: FTMS + c NSI d Full ms2 725.2885

100 200 300 400 500 600 700 800 900 1000 1100 1200 1300 1400 1500m/z

0

5

10

15

20

25

30

35

40

45

50

55

60

65

70

75

80

85

90

95

100

Rel

ativ

e A

bund

ance

258.0870z=?

189.0293z=?

286.1391z=?

173.0920z=?

440.2129z=1

86.0605z=?

155.0813z=?

343.1600z=?

509.1567z=?

663.2312z=1

610.1680z=1

726.7686z=2

845.2963z=1

930.3410z=?

1112.3971z=?

N

NN

NO

O

NHO

HO

O O

O

OH

HN

O

NH

NO2

20