Alterations in the Salivary Proteome and N ... - ACS Publications

Mar 10, 2017 - Katherine E. Williams, ... KEYWORDS: Sjögren's Syndrome, isobaric mass tagging, iTRAQ, lectin affinity capture, parotid saliva, whole ...
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Alterations in the Salivary Proteome and NGlycome of Sjögren’s Syndrome Patients Steven C. Hall, Maria E. Hassis, Katherine E Williams, Matthew E Albertolle, Akraporn Prakobphol, Andrew B Dykstra, Megan Laurance, Katherine Ona, Richard K. Niles, Namrata Prasad, Matthew Gormley, Caroline H Shiboski, Lindsey A. Criswell, H. Ewa Witkowska, and Susan J. Fisher J. Proteome Res., Just Accepted Manuscript • DOI: 10.1021/acs.jproteome.6b01051 • Publication Date (Web): 10 Mar 2017 Downloaded from http://pubs.acs.org on March 12, 2017

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Journal of Proteome Research is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties.

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FIGURES

Figure 1. Many of the differentially expressed salivary proteins in saliva samples from pSS patients and control individuals were unique to the donor group. Shown is the number of shared and unique proteins among the groups: pSS vs. HC, pSS vs. SC, and SC vs. HC. Data are shown for both saliva types PS (a) and WS (b) that were analyzed.



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b2M

1

2

3 4

5

6 7

8

9 10

17 Kd

b2-microglobulin, PS é

Relative Intensity

(a)

1.2 1 0.8 0.6 0.4 0.2 0 pSS

Healthy

1

2

3 4

5

6 7

8

9 10

70 Kd 55 Kd

Carbonic anhydrase VI, WS ê

Relative Intensity

CAH6 (b)

3 2.5 2 1.5 1 0.5 0 pSS

(c)

1

2

3 4

5

6 7

8

70 Kd 55 Kd

BPI fold-containing family B member 2, WS ê

Healthy

BPIFB2

9 10 Relative Intensity

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 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 60

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25 20 15 10 5 0 pSS

Healthy

Figure 2. Validation of the proteins identified as differentially expressed in the iTRAQ experiments. Immunoblotting was used to verify the iTRAQ results in an independent cohort of PS and WS samples collected from pSS and HC donors (n=5 per group). Overall, significantly higher amounts of b2-microglobulin were observed in pSS PS salivas as compared to HC samples (a), thus verifying the up-regulation detected in the iTRAQ experiment. Downregulation of carbonic anhydrase VI in PS (b) and BPI fold-containing family B member 2 in WS was also confirmed. Lanes 1-5: pSS, lanes 6-10: HC. Refer to Figure S-1 for images of the entire immunoblot.



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(a)

Figure 3. Ingenuity Pathway Analysis showed that the proteins, which were DE in Sjogren’s Syndrome pSS vs. HC for PS and WS samples, were networked with proteins that are involved in this disease and in psoriasis, another autoimmune condition. 1) salivary DE proteins (red, upregulated; blue down-regulated) identified in the iTRAQ analyses that are involved with psoriasis; 2) proteins associated with Sjögren’s Syndrome (purple outline); 3) direct (physical ± functional; solid lines) or indirect (functional; dashed lines) interactions; and 4) shapes outlining the protein names denote the family to which they belong (refer to Table S-6 for shape definitions). The results suggested that many of the observed alterations were networked with pivotal immune and signaling pathway that also implicated in the disease etiology of psoriasis.



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AAL

(a) Percent of Total N-Glycosites

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(b)

WGA

100

100

80

80

60

60

pSS

40

40

SC

20

20

HC

0

0

PS

WS

PS

WS

Figure 4. pSS is associated with increased N-glycosylation of salivary proteins. Shown is the percent of total N-glycosites observed in pSS, SC and HC pooled PS and WS samples. Chromatography on AAL (a) or WGA (b) captured the highest number of N-glycosites from pSS (blue) samples as compared to the SC (red) and HC (green) salivas. Overall, the HC group had the lowest number with SCs at an intermediate level. An exception was the WGA-bound fraction from WS in which the number of N-glycosites observed in the HC group was greater than the SC group.

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Table 1. Numbers of differentially expressed (p < 0.05) proteins observed in disease (pSS), SICCA control (SC) and healthy control (HC) salivas.

Saliva Type Parotid

pSS vs. HC

pSS vs. SC

SC vs. HC

 

44 23 21

20 11 9

27 14 13

 

49 21 28

21 10 11

17 3 14

Total

Whole

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Table 2a. iTRAQ-based comparison of relative abundances of proteins observed in PS and WS from pSS patients vs. healthy individuals. UniProt Accession Number P62805

Protein Name

Saliva Type

Histone H4

WS

1.1E-02

 9.6

Q6FI13

Histone H2A type 2-A

WS

1.8E-02

 8.4

Q5QNW6

Histone H2B type 2-F

WS

6.3E-04

 6.7

Q71DI3

Histone H3.2

WS

4.3E-02

 4.1

P61769

Beta-2-microglobulin

PS

1.5E-02

 4.1

P04083

Annexin A1

WS

1.1E-02

 3.7

Q08380

Galectin-3-binding protein

PS

1.0E-04

 2.8

Q96DR5

BPI fold-containing family A member

PS

6.9E-04

6.7

P23280-2

Isoform 2 of Carbonic anhydrase 6

WS

1.1E-03

7.7

P23280

Carbonic anhydrase 6

PS

7.6E-04

8.3

Q96DR5

BPI fold-containing family A member 2

WS

7.7E-04

9.1

Q8N4F0

BPI fold-containing family B member 2

WS

2.9E-05

10

Q8TDL5

BPI fold-containing family B member 1

WS

1.2E-05

14

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p-value

Fold Change

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Table 2b. iTRAQ-based comparison of relative abundances of proteins observed in PS and WS from pSS patients vs. SICCA controls. UniProt Accession Number Q6FI13

Protein Name

Saliva Type

Histone H2A type 2-A

WS

8.0E-03

 10

P01857

Ig gamma-1 chain C region

PS

1.6E-04

 9.5

Q92817

Envoplakin

WS

2.6E-02

 7.9

P62805

Histone H4

WS

2.4E-02

 6.7

Q15782

Chitinase-3-like protein 2

PS

2.7E-02

 5.7

P07476

Involucrin

PS

3.4E-02

 4.3

P63104

14-3-3 protein zeta/delta

PS

3.6E-02

 4.2

P05164

Myeloperoxidase

WS

3.5E-02

P06870

Kallikrein-1

WS PS

1.9E-02 1.5E-02

 3.4 4.0 4.1

P01877

Ig alpha-2 chain C region

WS

5.3E-03

4.3

Q96DR5

BPI fold-containing family A member 2

WS

3.4E-03

7.1

P23280 P23280-2

Carbonic anhydrase 6 Isoform 2 of Carbonic anhydrase 6

P15515

Histatin-1

PS WS PS WS

1.1E-02 4.8E-04 1.1E-02 5.2E-04

3.8 7.7 3.8 8.3

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Table 3. Glycoproteins detected in pSS, SC, and HC WS and PS saliva samples by lectin affinity capture with AAL and WGA lectins. Identification was made by MS. Accession numbers with an “*” indicate proteins that were not identified in the iTRAQ experiments. AAL Accession Number P01833 P01876 P01877 P02788 P04220* P22079 P25311 Q08380 P04745 P00738 P01033 P01871 P02787 P02790 P05164 P10909 P13646* P20061 P32926 P80188 Q02413 Q02487 Q9HC84 Q9UGM3 Q9Y6R7 P06870 Q8N4F0 P01009

Protein Name Polymeric immunoglobulin receptor Ig alpha-1 chain C region Ig alpha-2 chain C region Lactotransferrin Ig mu heavy chain disease protein Lactoperoxidase Zinc-alpha-2-glycoprotein Galectin-3-binding protein Alpha-amylase 1 Haptoglobin Metalloproteinase inhibitor 1 Ig mu chain C region Serotransferrin Hemopexin Myeloperoxidase Clusterin Keratin, type I cytoskeletal 13 Transcobalamin-1 Desmoglein-3 Neutrophil gelatinase-associated lipocalin Desmoglein-1 Desmocollin-2 Mucin-5B Deleted in malignant brain tumors 1 IgGFc-binding protein Kallikrein-1 BPI fold-containing family B member 2 Alpha-1-antitrypsin

Gene Name PIGR_HUMAN IGHA1_HUMAN IGHA2_HUMAN TRFL_HUMAN MUCB_HUMAN PERL_HUMAN ZA2G_HUMAN LG3BP_HUMAN AMY1_HUMAN HPT_HUMAN TIMP1_HUMAN IGHM_HUMAN TRFE_HUMAN HEMO_HUMAN PERM_HUMAN CLUS_HUMAN K1C13_HUMAN TCO1_HUMAN DSG3_HUMAN NGAL_HUMAN DSG1_HUMAN DSG2_HUMAN MUC5B_HUMAN DMBT1_HUMAN FCGBP_HUMAN KLK1_HUMAN BPIB2_HUMAN A1AT_HUMAN

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WGA

PS

WS

PS

WS

x x x x x x x x x

x x x x

x x x x

x x x x

x x x

x x x

x

x x x x x x x x x x x x x x x x x x

x x

x x

x

x

x x x x

x

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Table 4. WGA lectin affinity capture and MS identification of glycoproteins and N-glycosites from pSS, SC, and HC parotid saliva samples. pSS Accession Number P01009 P01833

Protein

Glycosite

SC

HC

Sequence*

Alpha-1-antitrypsin

A1AT_HUMAN@107

ADTHDEILEGLNFNLTEIPEAQIHEGFQELLR

x

Polymeric immunoglobulin receptor

PIGR_HUMAN@135 PIGR_HUMAN@186 PIGR_HUMAN@469 PIGR_HUMAN@83

GLSFDVSLEVSQGPGLLNDTK QIGLYPVLVIDSSGYVNPNYTGR VPGNVTAVLGETLK ANLTNFPENGTFVVNIAQLSQDDSGR

x x x x

x x x x

P01871

Ig mu chain C

IGHM_HUMAN@439

STGKPTLYNVSLVMSDTAGTCY

x

P01876

Ig alpha-1 chain C

IGHA1_HUMAN@144 IGHA1_HUMAN@340

HRPALEDLLLGSEANLTCTLTGLR LAGKPTHVNVSVVMAEVDGTCY

x x

x x

P01877

Ig alpha-2 chain C region

IGHA2_HUMAN@131 IGHA2_HUMAN@327 IGHA2_HUMAN@47

HRPALEDLLLGSEANLTCTLTGLR PTHVNVSVVMAEVDGTCY LVQGFFPQEPLSVTWSESGQNVTAR

x x x

x x x

P02788

Lactotransferrin

TRFL_HUMAN@156 TRFL_HUMAN@497

PFLNWTGPPEPIEAAVAR TAGWNIPMGLLFNQTGSCK

x x

P10909

Clusterin

CLUS_HUMAN@354 CLUS_HUMAN@374

MLNTSSLLEQLNEQFNWVSR LANLTQGEDQYYLR

x x

P22079

Lactoperoxidase

PERL_HUMAN@106

ASLTNVTDPSLDLTSLSLEVGCGAPAPVVR

x

x

P25311

Zinc-alpha-2-glycoprotein

ZA2G_HUMAN@109

DIVEYYNDSNGSHVLQGR

x

x

P80188

Neutrophil gelatinase-associated lipocalin

NGAL_HUMAN@85

SYNVTSVLFR

x

Q08380

Galectin-3-binding protein

LG3BP_HUMAN@69

ALGFENATQALGR

x

* The consensus sequence is highlighted in red.

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x x

x x

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Author Names and Affiliations Name Steven C. Hall

Affiliation Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA Sandler-Moore Mass Spectrometry Core Facility, University of California, San Francisco, San Francisco, CA 94143, USA

Maria E. Hassis

Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA Sandler-Moore Mass Spectrometry Core Facility, University of California, San Francisco, San Francisco, CA 94143, USA

Katherine E. Williams

Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA Sandler-Moore Mass Spectrometry Core Facility, University of California, San Francisco, San Francisco, CA 94143, USA

Matthew E. Albertolle

Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA Sandler-Moore Mass Spectrometry Core Facility, University of California, San Francisco, San Francisco, CA 94143, USA

Akraporn Prakobphol

Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA

Andrew B. Dykstra

Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA Sandler-Moore Mass Spectrometry Core Facility, University of California, San Francisco, San Francisco, CA 94143, USA

Megan Laurance

Library and Center for Knowledge Management, University of California, San Francisco, San Francisco, California, 94143, USA

Katherine Ona

Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA

Richard K. Niles

Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA Sandler-Moore Mass Spectrometry Core Facility, University of California, San Francisco, San Francisco, CA 94143, USA

Narmrata Prasad

Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA Sandler-Moore Mass Spectrometry Core Facility, University of California, San Francisco, San Francisco, CA 94143, USA

Matthew Gormley

Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA

Caroline Shiboski

Department of Orofacial Sciences, University of California, San Francisco, California, 94143, USA

Lindsey A. Criswell

Department of Orofacial Sciences, University of California, San Francisco, California, 94143, USA Russel / Engleman Rheumatology Research Center, Department of Medicine, University of California, San Francisco, San Francisco, California, 94143, USA

H. Ewa Witkowska

Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA Sandler-Moore Mass Spectrometry Core Facility, University of California, San Francisco, San Francisco, CA 94143, USA

Susan J. Fisher

Department of Obstetrics, Gynecology and Reproductive Sciences, University of California, San Francisco, San Francisco, California, 94143, USA Sandler-Moore Mass Spectrometry Core Facility, University of California, San Francisco, San Francisco, CA 94143, USA

Article Title Alterations in the Salivary Proteome and N-Glycome of Sjögren’s Syndrome Patients

Item Figure S-1 Table S-1 Table S-2 Table S-3 Table S-4 Table S-5 Table S-6

Table of Contents Content Whole image immunoblots for validation of iTRAQ DE proteins. Parotid and whole salivary proteins identified and quantified in the iTRAQ experiment at an FDR of 5% Comparison of differentially expressed proteins among donor groups (p < 0.05) WGA lectin affinity capture and MS identification of glycoproteins and N-glycosites from pSS, SC, and HC whole saliva samples AAL lectin affinity capture and MS identification of glycoproteins and N-glycosites from pSS, SC, and HC parotid saliva samples AAL lectin affinity capture and MS identification of glycoproteins and N-glycosites from pSS, SC, and HC whole saliva samples Legend matching shapes to protein families for Figures 3a and 3b.

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Figure S-1. Whole image immunoblots for validation of iTRAQ DE proteins. (a) beta-2-microglobulin was up-regulated in PS while (b) carbonic anhydrase VI in WS and © BPI fold-containing family B member 2 in WS were down regulated, respectively from pSS pactients compared to HCs

(a)

(b)

(c)

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1 Table S-1. Parotid and whole salivary proteins identified and quantified in the iTRAQ experiment at an FDR of 5%. 2 3 Parotid Saliva pSS / HC pSS / HC pSS / HC pSS / HC pSS / SC pSS / SC Accession Number and Gene Name Protein Name ttest fold lin fold log n1-n2 ttest fold lin 4 Master N 1 sp|P04745|AMY1_HUMAN Alpha-amylase 1 OS=Homo sapiens GN=AMY1A PE=1 SV=2 2.9E-03 0.80 -0.10 15:15 3.6E-02 0.85 2 sp|P02810|PRPC_HUMAN Salivary acidic proline-rich phosphoprotein 1/2 OS=Homo sapiens GN=PRH1 PE=1 SV=2 4.7E-02 0.54 -0.27 15:15 3.0E-01 0.76 5 3 sp|P02812|PRB2_HUMAN Basic salivary proline-rich protein 2 OS=Homo sapiens GN=PRB2 PE=1 SV=3 1.2E-01 0.30 -0.52 15:15 8.8E-02 0.28 4 sp|P01876|IGHA1_HUMAN Ig alpha-1 chain C region OS=Homo sapiens GN=IGHA1 PE=1 SV=2 4.3E-01 1.41 0.15 15:15 6.5E-01 0.79 6 5 sp|P01833|PIGR_HUMAN Polymeric immunoglobulin receptor OS=Homo sapiens GN=PIGR PE=1 SV=4 1.6E-02 2.39 0.38 15:15 6.0E-01 0.82 6 sp|P02788|TRFL_HUMAN Lactotransferrin OS=Homo sapiens GN=LTF PE=1 SV=6 2.2E-02 2.11 0.32 15:15 2.1E-02 1.74 7 7 sp|P02768|ALBU_HUMAN Serum albumin OS=Homo sapiens GN=ALB PE=1 SV=2 4.6E-01 1.38 0.14 15:15 7.9E-01 0.91 8 sp|P04280|PRP1_HUMAN Basic salivary proline-rich protein 1 OS=Homo sapiens GN=PRB1 PE=1 SV=2 8.4E-01 0.83 -0.08 15:15 3.9E-01 0.47 8 9 sp|P02814|SMR3B_HUMAN Submaxillary gland androgen-regulated protein 3B OS=Homo sapiens GN=SMR3B PE=1 SV=2 9.2E-01 1.05 0.02 15:15 9.8E-01 1.01 10 sp|P22079|PERL_HUMAN Lactoperoxidase OS=Homo sapiens GN=LPO PE=1 SV=2 7.7E-03 0.42 -0.38 15:15 4.5E-01 0.76 9 11 sp|Q9UGM3-5|DMBT1_HUMAN Isoform 5 of Deleted in malignant brain tumors 1 protein OS=Homo sapiens GN=DMBT1 2.1E-01 1.45 0.16 15:15 9.1E-01 0.96 12 sp|P25311|ZA2G_HUMAN Zinc-alpha-2-glycoprotein OS=Homo sapiens GN=AZGP1 PE=1 SV=2 9.1E-01 1.03 0.01 15:15 5.7E-02 0.60 10 13 sp|P23280|CAH6_HUMAN Carbonic anhydrase 6 OS=Homo sapiens GN=CA6 PE=1 SV=3 7.6E-04 0.12 -0.91 11:10 1.1E-02 0.26 14 sp|P10163|PRB4_HUMAN Basic salivary proline-rich protein 4 OS=Homo sapiens GN=PRB4 PE=1 SV=3 5.4E-01 0.36 -0.44 3:5 4.3E-01 0.26 11 15 sp|P02787|TRFE_HUMAN Serotransferrin OS=Homo sapiens GN=TF PE=1 SV=3 9.9E-03 2.42 0.38 15:15 1.4E-02 2.42 16 sp|P61626|LYSC_HUMAN Lysozyme C OS=Homo sapiens GN=LYZ PE=1 SV=1 1.3E-01 1.72 0.24 15:15 6.7E-01 1.13 12 17 sp|P01857|IGHG1_HUMAN Ig gamma-1 chain C region OS=Homo sapiens GN=IGHG1 PE=1 SV=1 7.7E-04 6.20 0.79 15:15 1.6E-04 9.49 18 sp|P01834|IGKC_HUMAN Ig kappa chain C region OS=Homo sapiens GN=IGKC PE=1 SV=1 1.8E-03 3.52 0.55 15:15 4.8E-01 1.28 13 19 sp|P04264|K2C1_HUMAN Keratin, type II cytoskeletal 1 OS=Homo sapiens GN=KRT1 PE=1 SV=6 9.2E-02 0.50 -0.30 15:15 5.9E-02 0.40 20 sp|P01871|IGHM_HUMAN Ig mu chain C region OS=Homo sapiens GN=IGHM PE=1 SV=3 3.2E-03 3.15 0.50 15:15 4.0E-01 1.33 21 sp|P13645|K1C10_HUMAN Keratin, type I cytoskeletal 10 OS=Homo sapiens GN=KRT10 PE=1 SV=6 3.1E-02 0.42 -0.38 15:15 1.9E-01 0.54 14 22 sp|P12273|PIP_HUMAN Prolactin-inducible protein OS=Homo sapiens GN=PIP PE=1 SV=1 5.8E-01 1.22 0.09 15:15 3.8E-01 1.35 23 sp|P18136|KV313_HUMAN Ig kappa chain V-III region HIC OS=Homo sapiens PE=2 SV=2 2.6E-01 1.41 0.15 15:15 8.3E-01 0.94 15 24 sp|P0CG05|LAC2_HUMAN Ig lambda-2 chain C regions OS=Homo sapiens GN=IGLC2 PE=1 SV=1 1.3E-09 5.33 0.73 15:15 5.5E-01 1.13 25 sp|P01877|IGHA2_HUMAN Ig alpha-2 chain C region OS=Homo sapiens GN=IGHA2 PE=1 SV=3 2.1E-01 0.59 -0.23 15:15 9.1E-03 0.33 16 26 sp|P10909-2|CLUS_HUMAN Isoform 2 of Clusterin OS=Homo sapiens GN=CLU 1.1E-03 2.28 0.36 15:15 2.7E-03 2.45 27 sp|Q96DR5|BPIA2_HUMAN BPI fold-containing family A member 2 OS=Homo sapiens GN=BPIFA2 PE=1 SV=2 6.9E-04 0.15 -0.84 15:15 2.3E-01 0.53 17 28 sp|P06870|KLK1_HUMAN Kallikrein-1 OS=Homo sapiens GN=KLK1 PE=1 SV=2 4.8E-01 0.66 -0.18 15:15 1.6E-02 0.24 29 sp|P15515|HIS1_HUMAN Histatin-1 OS=Homo sapiens GN=HTN1 PE=1 SV=2 3.1E-04 0.16 -0.80 15:15 1.5E-02 0.26 18 30 sp|P01591|IGJ_HUMAN Immunoglobulin J chain OS=Homo sapiens GN=IGJ PE=1 SV=4 5.5E-03 2.30 0.36 15:15 8.0E-01 0.94 31 sp|Q96DA0|ZG16B_HUMAN Zymogen granule protein 16 homolog B OS=Homo sapiens GN=ZG16B PE=1 SV=3 9.7E-01 1.02 0.01 15:15 3.6E-01 1.58 19 32 sp|P01023|A2MG_HUMAN Alpha-2-macroglobulin OS=Homo sapiens GN=A2M PE=1 SV=3 5.1E-01 3.77 0.58 2:2 5.7E-01 3.12 33 sp|Q9UBC9|SPRR3_HUMAN Small proline-rich protein 3 OS=Homo sapiens GN=SPRR3 PE=1 SV=2 8.3E-04 0.12 -0.92 14:12 2.1E-01 0.48 20 34 sp|P01009|A1AT_HUMAN Alpha-1-antitrypsin OS=Homo sapiens GN=SERPINA1 PE=1 SV=3 3.5E-02 3.36 0.53 15:15 4.1E-01 1.39 35 sp|P01024|CO3_HUMAN Complement C3 OS=Homo sapiens GN=C3 PE=1 SV=2 1.2E-01 1.92 0.28 15:15 5.1E-02 2.22 21 36 sp|P09228|CYTT_HUMAN Cystatin-SA OS=Homo sapiens GN=CST2 PE=1 SV=1 1.4E-01 0.61 -0.22 15:15 9.3E-01 1.03 37 sp|P63261|ACTG_HUMAN Actin, cytoplasmic 2 OS=Homo sapiens GN=ACTG1 PE=1 SV=1 4.3E-01 2.36 0.37 6:6 3.7E-01 2.12 22 38 sp|P01766|HV305_HUMAN Ig heavy chain V-III region BRO OS=Homo sapiens PE=1 SV=1 2.8E-01 0.68 -0.17 15:15 1.8E-01 0.61 39 sp|P02647|APOA1_HUMAN Apolipoprotein A-I OS=Homo sapiens GN=APOA1 PE=1 SV=1 1.9E-01 10.42 1.02 2:2 2.7E-01 10.96 23 40 sp|P28325|CYTD_HUMAN Cystatin-D OS=Homo sapiens GN=CST5 PE=1 SV=1 3.4E-01 0.61 -0.22 15:15 6.3E-01 1.32 41 sp|P01034|CYTC_HUMAN Cystatin-C OS=Homo sapiens GN=CST3 PE=1 SV=1 3.5E-01 0.72 -0.14 15:15 6.2E-01 1.20 24 42 sp|Q08380|LG3BP_HUMAN Galectin-3-binding protein OS=Homo sapiens GN=LGALS3BP PE=1 SV=1 1.0E-04 2.81 0.45 15:15 2.3E-02 1.67 43 sp|P02808|STAT_HUMAN Statherin OS=Homo sapiens GN=STATH PE=1 SV=2 2.8E-02 0.50 -0.30 13:13 3.9E-01 0.76 25 44 sp|Q8TDL5|BPIB1_HUMAN BPI fold-containing family B member 1 OS=Homo sapiens GN=BPIFB1 PE=2 SV=1 1.6E-02 0.41 -0.39 15:15 1.5E-01 0.58 45 sp|Q02818|NUCB1_HUMAN Nucleobindin-1 OS=Homo sapiens GN=NUCB1 PE=1 SV=4 2.2E-01 0.50 -0.30 10:11 5.4E-01 0.66 46 sp|P35908|K22E_HUMAN Keratin, type II cytoskeletal 2 epidermal OS=Homo sapiens GN=KRT2 PE=1 SV=2 3.2E-02 0.41 -0.39 15:15 8.3E-02 0.45 26 47 sp|P35527|K1C9_HUMAN Keratin, type I cytoskeletal 9 OS=Homo sapiens GN=KRT9 PE=1 SV=3 3.0E-01 0.64 -0.19 15:15 4.7E-02 0.45 48 sp|P80303|NUCB2_HUMAN Nucleobindin-2 OS=Homo sapiens GN=NUCB2 PE=1 SV=2 3.9E-02 0.44 -0.36 15:15 7.3E-01 0.86 27 49 sp|P0C0L4-2|CO4A_HUMAN Isoform 2 of Complement C4-A OS=Homo sapiens GN=C4A 7.6E-01 0.90 -0.05 9:8 5.4E-01 1.31 50 sp|Q16378|PROL4_HUMAN Proline-rich protein 4 OS=Homo sapiens GN=PRR4 PE=1 SV=3 1.0E-01 0.34 -0.47 15:15 7.0E-01 0.80 28 51 sp|P01037|CYTN_HUMAN Cystatin-SN OS=Homo sapiens GN=CST1 PE=1 SV=3 7.8E-01 0.88 -0.06 15:15 2.2E-01 1.74 52 sp|P00450|CERU_HUMAN Ceruloplasmin OS=Homo sapiens GN=CP PE=1 SV=1 7.1E-01 1.30 0.11 5:4 8.8E-01 1.12 29 53 sp|P04083|ANXA1_HUMAN Annexin A1 OS=Homo sapiens GN=ANXA1 PE=1 SV=2 3.7E-01 0.65 -0.19 15:15 9.7E-01 0.98 54 sp|P03973|SLPI_HUMAN Antileukoproteinase OS=Homo sapiens GN=SLPI PE=1 SV=2 5.7E-01 0.79 -0.10 15:15 1.8E-01 0.58 30 55 sp|P04080|CYTB_HUMAN Cystatin-B OS=Homo sapiens GN=CSTB PE=1 SV=2 6.7E-03 0.27 -0.56 15:15 6.3E-01 1.25 56 sp|P02774|VTDB_HUMAN Vitamin D-binding protein OS=Homo sapiens GN=GC PE=1 SV=1 7.1E-01 1.27 0.10 10:8 5.2E-01 0.66 31 57 sp|P02533|K1C14_HUMAN Keratin, type I cytoskeletal 14 OS=Homo sapiens GN=KRT14 PE=1 SV=4 4.6E-01 1.40 0.15 11:11 4.3E-01 1.71 58 sp|P07339|CATD_HUMAN Cathepsin D OS=Homo sapiens GN=CTSD PE=1 SV=1 6.1E-01 1.16 0.06 12:13 9.0E-01 0.97 32 59 sp|P04207|KV308_HUMAN Ig kappa chain V-III region CLL OS=Homo sapiens PE=1 SV=2 9.0E-02 1.74 0.24 6:7 9.4E-01 0.98 60 sp|P07602-3|SAP_HUMAN Isoform Sap-mu-9 of Proactivator polypeptide OS=Homo sapiens GN=PSAP 3.0E-01 1.37 0.14 15:15 2.1E-01 1.41 33 61 sp|P80188|NGAL_HUMAN Neutrophil gelatinase-associated lipocalin OS=Homo sapiens GN=LCN2 PE=1 SV=2 1.1E-02 2.72 0.43 15:15 3.2E-02 2.40 62 sp|P07237|PDIA1_HUMAN Protein disulfide-isomerase OS=Homo sapiens GN=P4HB PE=1 SV=3 1.8E-02 0.40 -0.39 10:11 5.2E-01 0.77 34 63 sp|P00738|HPT_HUMAN Haptoglobin OS=Homo sapiens GN=HP PE=1 SV=1 2.4E-01 2.37 0.37 7:6 3.8E-01 2.00 64 sp|P01011|AACT_HUMAN Alpha-1-antichymotrypsin OS=Homo sapiens GN=SERPINA3 PE=1 SV=2 4.4E-02 2.79 0.45 12:10 4.5E-01 1.25 35 65 sp|P00751|CFAB_HUMAN Complement factor B OS=Homo sapiens GN=CFB PE=1 SV=2 5.5E-01 1.58 0.20 7:6 5.3E-01 1.76 66 sp|P02790|HEMO_HUMAN Hemopexin OS=Homo sapiens GN=HPX PE=1 SV=2 4.3E-01 2.35 0.37 10:8 2.1E-01 3.68 36 67 sp|Q14508|WFDC2_HUMAN WAP four-disulfide core domain protein 2 OS=Homo sapiens GN=WFDC2 PE=1 SV=2 3.2E-02 2.09 0.32 15:15 9.1E-01 0.97 68 sp|P06309|KV205_HUMAN Ig kappa chain V-II region GM607 (Fragment) OS=Homo sapiens PE=4 SV=1 7.3E-03 2.43 0.39 15:15 6.0E-01 1.18 37 69 sp|P06733|ENOA_HUMAN Alpha-enolase OS=Homo sapiens GN=ENO1 PE=1 SV=2 4.5E-01 0.78 -0.11 9:8 3.0E-01 1.62 70 sp|P01743|HV102_HUMAN Ig heavy chain V-I region HG3 OS=Homo sapiens PE=4 SV=1 1.3E-01 1.99 0.30 13:13 5.1E-01 0.76 71 sp|P01860|IGHG3_HUMAN Ig gamma-3 chain C region OS=Homo sapiens GN=IGHG3 PE=1 SV=2 1.6E-01 2.87 0.46 8:9 1.0E-01 5.12 38 72 sp|P01714|LV301_HUMAN Ig lambda chain V-III region SH OS=Homo sapiens PE=1 SV=1 2.0E-01 2.33 0.37 15:15 3.8E-01 1.69 73 sp|Q9HC84|MUC5B_HUMAN Mucin-5B OS=Homo sapiens GN=MUC5B PE=1 SV=3 1.7E-01 0.70 -0.15 11:11 4.4E-01 1.23 39 74 sp|B9A064|IGLL5_HUMAN Immunoglobulin lambda-like polypeptide 5 OS=Homo sapiens GN=IGLL5 PE=2 SV=2 8.7E-04 2.98 0.47 15:15 6.8E-01 0.90 75 sp|P05109|S10A8_HUMAN Protein S100-A8 OS=Homo sapiens GN=S100A8 PE=1 SV=1 7.2E-01 0.84 -0.08 15:15 8.8E-02 2.80 40 76 sp|P01609|KV117_HUMAN Ig kappa chain V-I region Scw OS=Homo sapiens PE=1 SV=1 4.3E-02 0.44 -0.36 8:9 3.4E-02 0.37 77 sp|P52209|6PGD_HUMAN 6-phosphogluconate dehydrogenase, decarboxylating OS=Homo sapiens GN=PGD PE=1 SV=3 4.1E-02 0.49 -0.31 7:6 6.2E-01 1.19 41 78 sp|P01781|HV320_HUMAN Ig heavy chain V-III region GAL OS=Homo sapiens PE=1 SV=1 5.1E-01 1.30 0.11 15:15 8.2E-01 0.90 79 sp|P08123|CO1A2_HUMAN Collagen alpha-2(I) chain OS=Homo sapiens GN=COL1A2 PE=1 SV=7 2.6E-02 0.37 -0.43 6:7 1.0E+00 1.00 42 80 sp|P07996|TSP1_HUMAN Thrombospondin-1 OS=Homo sapiens GN=THBS1 PE=1 SV=2 7.6E-01 1.18 0.07 5:4 6.2E-01 1.56 81 sp|P23284|PPIB_HUMAN Peptidyl-prolyl cis-trans isomerase B OS=Homo sapiens GN=PPIB PE=1 SV=2 2.4E-02 0.45 -0.34 15:15 3.2E-01 0.70 43 82 sp|P80748|LV302_HUMAN Ig lambda chain V-III region LOI OS=Homo sapiens PE=1 SV=1 4.6E-01 1.54 0.19 15:15 7.4E-01 1.24 83 sp|A8K2U0|A2ML1_HUMAN Alpha-2-macroglobulin-like protein 1 OS=Homo sapiens GN=A2ML1 PE=1 SV=3 2.4E-01 0.57 -0.25 5:4 7.9E-01 1.06 44 84 sp|P08107|HSP71_HUMAN Heat shock 70 kDa protein 1A/1B OS=Homo sapiens GN=HSPA1A PE=1 SV=5 3.8E-01 0.50 -0.30 5:4 6.2E-01 0.57 85 sp|P06702|S10A9_HUMAN Protein S100-A9 OS=Homo sapiens GN=S100A9 PE=1 SV=1 4.8E-01 1.84 0.26 7:6 1.1E-01 8.16 45 86 sp|P04406|G3P_HUMAN Glyceraldehyde-3-phosphate dehydrogenase OS=Homo sapiens GN=GAPDH PE=1 SV=3 9.0E-01 0.95 -0.02 15:15 2.9E-01 1.46 87 sp|Q9H4L7-3|SMRCD_HUMAN Isoform 3 of SWI/SNF-related matrix-associated actin-dependent regulator of chromatin subfamily A containing DEAD/H box 1 OS=Homo sapiens GN=SMARCAD1 1.6E-01 0.39 -0.41 3:5 1.9E-01 0.39 46 88 sp|P01772|HV311_HUMAN Ig heavy chain V-III region KOL OS=Homo sapiens PE=1 SV=1 89 sp|P68871|HBB_HUMAN Hemoglobin subunit beta OS=Homo sapiens GN=HBB PE=1 SV=2 9.7E-01 0.96 -0.02 4:4 2.8E-01 3.39 47 90 sp|P01602|KV110_HUMAN Ig kappa chain V-I region HK102 (Fragment) OS=Homo sapiens GN=IGKV1-5 PE=4 SV=1 7.8E-01 1.06 0.03 15:15 8.0E-01 1.07 91 sp|Q96RW7-2|HMCN1_HUMAN Isoform 2 of Hemicentin-1 OS=Homo sapiens GN=HMCN1 3.3E-01 0.26 -0.58 2:2 3.0E-01 0.25 48 92 sp|P07476|INVO_HUMAN Involucrin OS=Homo sapiens GN=IVL PE=1 SV=2 1.5E-01 0.53 -0.27 8:6 3.4E-02 4.29 93 sp|P06396|GELS_HUMAN Gelsolin OS=Homo sapiens GN=GSN PE=1 SV=1 7.4E-01 1.25 0.10 10:8 8.9E-01 1.10 49 94 sp|P01764|HV303_HUMAN Ig heavy chain V-III region VH26 OS=Homo sapiens PE=1 SV=1 1.8E-01 0.70 -0.16 15:15 3.9E-03 0.45 95 sp|P10599-2|THIO_HUMAN Isoform 2 of Thioredoxin OS=Homo sapiens GN=TXN 7.4E-02 0.48 -0.32 14:12 6.4E-01 1.21 96 sp|P28799|GRN_HUMAN Granulins OS=Homo sapiens GN=GRN PE=1 SV=2 1.4E-01 1.46 0.16 5:4 3.8E-01 1.45 50 97 sp|P61769|B2MG_HUMAN Beta-2-microglobulin OS=Homo sapiens GN=B2M PE=1 SV=1 1.5E-02 4.05 0.61 10:11 1.5E-02 2.13 98 sp|P04433|KV309_HUMAN Ig kappa chain V-III region VG (Fragment) OS=Homo sapiens PE=1 SV=1 1.1E-02 3.05 0.48 15:15 2.4E-01 1.65 51 99 sp|P06314|KV404_HUMAN Ig kappa chain V-IV region B17 OS=Homo sapiens PE=2 SV=1 7.8E-01 1.09 0.04 15:15 3.7E-01 0.81 100 sp|P14618-2|KPYM_HUMAN Isoform M1 of Pyruvate kinase PKM OS=Homo sapiens GN=PKM 4.8E-01 1.30 0.11 5:4 1.4E-01 1.79 52 101 sp|P62158|CALM_HUMAN Calmodulin OS=Homo sapiens GN=CALM1 PE=1 SV=2 4.3E-01 0.71 -0.15 7:6 6.8E-01 0.84 102 sp|P30044|PRDX5_HUMAN Peroxiredoxin-5, mitochondrial OS=Homo sapiens GN=PRDX5 PE=1 SV=4 1.7E-01 0.59 -0.23 7:6 6.3E-01 0.79 53 103 sp|Q16651|PRSS8_HUMAN Prostasin OS=Homo sapiens GN=PRSS8 PE=1 SV=1 3.4E-01 1.37 0.14 5:4 9.0E-01 0.96 104 sp|P04075-2|ALDOA_HUMAN Isoform 2 of Fructose-bisphosphate aldolase A OS=Homo sapiens GN=ALDOA 7.9E-01 0.93 -0.03 3:2 0.96 54 105 sp|P08571|CD14_HUMAN Monocyte differentiation antigen CD14 OS=Homo sapiens GN=CD14 PE=1 SV=2 9.1E-01 1.03 0.01 15:15 7.8E-01 1.10 106 sp|P19013|K2C4_HUMAN Keratin, type II cytoskeletal 4 OS=Homo sapiens GN=KRT4 PE=1 SV=4 3.8E-01 0.40 -0.39 5:4 2.0E-01 0.22 55 107 sp|P20061|TCO1_HUMAN Transcobalamin-1 OS=Homo sapiens GN=TCN1 PE=1 SV=2 6.9E-01 1.35 0.13 5:4 3.5E-01 3.53 108 sp|P01019|ANGT_HUMAN Angiotensinogen OS=Homo sapiens GN=AGT PE=1 SV=1 4.2E-01 3.22 0.51 2:2 4.2E-01 2.54 56 109 sp|P15328|FOLR1_HUMAN Folate receptor alpha OS=Homo sapiens GN=FOLR1 PE=1 SV=3 7.1E-01 0.81 -0.09 6:7 1.0E-01 0.34 110 sp|P01717|LV403_HUMAN Ig lambda chain V-IV region Hil OS=Homo sapiens PE=1 SV=1 1.9E-01 0.67 -0.17 15:15 4.6E-01 0.78 57 111 sp|P04004|VTNC_HUMAN Vitronectin OS=Homo sapiens GN=VTN PE=1 SV=1 8.2E-01 1.40 0.15 7:6 6.5E-01 0.51 112 sp|P01008|ANT3_HUMAN Antithrombin-III OS=Homo sapiens GN=SERPINC1 PE=1 SV=1 6.4E-01 1.36 0.13 2:2 9.8E-01 0.98 58 113 sp|O00391|QSOX1_HUMAN Sulfhydryl oxidase 1 OS=Homo sapiens GN=QSOX1 PE=1 SV=3 6.7E-01 0.85 -0.07 7:7 6.6E-01 1.13 114 sp|P62937|PPIA_HUMAN Peptidyl-prolyl cis-trans isomerase A OS=Homo sapiens GN=PPIA PE=1 SV=2 6.4E-01 1.24 0.09 2:2 5.8E-01 1.29 59 115 sp|P04208|LV106_HUMAN Ig lambda chain V-I region WAH OS=Homo sapiens PE=1 SV=1 7.4E-03 3.53 0.55 15:15 7.0E-01 0.88 60 ACS Paragon Plus Environment

Page 12 of 26

pSS / SC pSS / SC SC / HC fold log n1-n2 ttest

SC / HC fold lin

SC / HC SC / HC fold log n1-n2

-0.07 -0.12 -0.55 -0.10 -0.09 0.24 -0.04 -0.33 0.00 -0.12 -0.02 -0.22 -0.59 -0.58 0.38 0.05 0.98 0.11 -0.39 0.12 -0.27 0.13 -0.03 0.05 -0.48 0.39 -0.28 -0.63 -0.58 -0.03 0.20 0.49 -0.32 0.14 0.35 0.01 0.33 -0.22 1.04 0.12 0.08 0.22 -0.12 -0.24 -0.18 -0.35 -0.34 -0.06 0.12 -0.10 0.24 0.05 -0.01 -0.24 0.10 -0.18 0.23 -0.02 -0.01 0.15 0.38 -0.11 0.30 0.10 0.25 0.57 -0.01 0.07 0.21 -0.12 0.71 0.23 0.09 -0.05 0.45 -0.43 0.08 -0.05 0.00 0.19 -0.16 0.09 0.03 -0.25 0.91 0.17 -0.41

15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 11:10 3:5 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 15:14 2:2 14:11 15:14 15:14 15:14 6:6 15:14 2:2 15:14 15:14 15:14 13:12 15:14 10:10 15:14 15:14 15:14 9:7 15:14 15:14 5:3 15:14 15:14 15:14 10:7 11:10 12:12 6:7 15:14 15:14 10:10 7:5 12:9 7:5 10:7 15:14 15:14 9:7 13:12 8:9 15:14 11:10 15:14 15:14 8:8 7:5 15:14 6:6 5:3 15:14 15:14 5:3 5:3 7:5 15:14 3:5

3.0E-01 1.9E-01 9.3E-01 2.1E-01 2.5E-03 5.8E-01 3.5E-01 5.4E-01 9.4E-01 2.5E-02 1.4E-01 3.1E-02 9.2E-03 8.0E-01 9.9E-01 2.2E-01 3.1E-01 1.5E-02 6.4E-01 2.2E-02 5.9E-01 7.7E-01 1.6E-01 3.4E-06 5.1E-02 7.9E-01 1.3E-03 2.2E-02 1.1E-01 2.5E-03 2.2E-01 8.1E-01 5.3E-02 1.3E-01 7.0E-01 1.8E-01 9.2E-01 7.2E-01 9.7E-01 2.1E-01 1.1E-01 3.8E-02 1.5E-01 3.2E-01 6.0E-01 8.3E-01 4.5E-01 2.7E-02 4.0E-01 2.0E-01 1.8E-01 7.9E-01 4.7E-01 3.0E-01 4.4E-03 2.7E-01 7.2E-01 5.8E-01 7.9E-02 9.2E-01 7.9E-01 2.2E-02 8.1E-01 1.4E-01 8.7E-01 7.0E-01 2.6E-02 1.8E-02 1.1E-01 4.0E-02 5.1E-01 6.2E-01 7.1E-02 6.5E-04 2.2E-02 7.0E-01 1.2E-02 3.9E-01 1.4E-02 7.6E-01 1.1E-01 7.2E-01 3.2E-01 9.2E-01 2.7E-01 2.8E-01 9.8E-01

0.95 0.71 1.05 1.78 2.93 1.21 1.53 1.78 1.04 0.55 1.51 1.71 0.48 1.39 1.00 1.52 0.65 2.75 1.23 2.37 0.78 0.90 1.50 4.69 1.80 0.93 0.28 2.81 0.61 2.45 0.65 1.21 0.25 2.42 0.87 0.59 1.11 1.12 0.95 0.46 0.60 1.68 0.66 0.71 0.76 0.91 1.42 0.51 0.69 0.42 0.51 1.16 0.66 1.37 0.22 1.92 0.82 1.20 1.77 0.97 1.13 0.53 1.18 2.23 0.90 0.64 2.16 2.05 0.48 2.63 0.56 1.38 0.57 3.32 0.30 1.18 0.41 1.45 0.37 0.75 0.65 1.24 0.53 0.87 0.23 0.65 0.99

-0.02 -0.15 0.02 0.25 0.47 0.08 0.18 0.25 0.02 -0.26 0.18 0.23 -0.31 0.14 0.00 0.18 -0.18 0.44 0.09 0.37 -0.11 -0.04 0.18 0.67 0.25 -0.03 -0.56 0.45 -0.21 0.39 -0.19 0.08 -0.60 0.38 -0.06 -0.23 0.05 0.05 -0.02 -0.34 -0.22 0.22 -0.18 -0.15 -0.12 -0.04 0.15 -0.30 -0.16 -0.37 -0.30 0.06 -0.18 0.14 -0.66 0.28 -0.09 0.08 0.25 -0.01 0.05 -0.28 0.07 0.35 -0.05 -0.19 0.33 0.31 -0.32 0.42 -0.25 0.14 -0.24 0.52 -0.53 0.07 -0.39 0.16 -0.43 -0.12 -0.19 0.10 -0.27 -0.06 -0.65 -0.19 -0.01

14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 10:10 5:5 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 14:15 2:2 11:12 14:15 14:15 14:15 6:6 14:15 2:2 14:15 14:15 14:15 12:13 14:15 10:11 14:15 14:15 14:15 7:8 14:15 14:15 3:4 14:15 14:15 14:15 7:8 10:11 12:13 7:7 14:15 14:15 10:11 5:6 9:10 5:6 7:8 14:15 14:15 7:8 12:13 9:9 14:15 10:11 14:15 14:15 8:9 5:6 14:15 6:7 3:4 14:15 14:15 3:4 3:4 5:6 14:15 5:5

0.53 0.03 -0.60 0.63 0.04 -0.34 0.08 0.16 0.33 0.22 -0.09 0.25 -0.07 -0.10 -0.02 -0.02 0.04 -0.66 0.55 0.40 -0.47 -0.11 -0.29 -0.01 0.05 0.11 -0.05

4:4 15:14 2:2 8:5 10:7 15:14 14:11 5:3 10:10 15:14 15:14 5:3 7:5 7:5 5:3 3:1 15:14 5:3 5:3 2:2 6:6 15:14 7:5 2:2 7:6 2:2 15:14

1.1E-01 9.8E-01 9.5E-01 1.8E-02 8.4E-01 6.2E-02 8.2E-02 9.9E-01 2.4E-01 8.3E-02 3.0E-01 5.3E-01 7.6E-01 6.0E-01 1.4E-01

0.28 0.99 1.04 0.12 1.14 1.54 0.39 1.00 1.90 1.84 1.35 0.73 0.84 0.75 1.44 0.97 0.94 1.86 0.38 1.27 2.37 0.86 2.74 1.38 0.75 0.96 4.00

-0.55 0.00 0.02 -0.90 0.06 0.19 -0.41 0.00 0.28 0.27 0.13 -0.14 -0.08 -0.13 0.16 -0.01 -0.03 0.27 -0.42 0.10 0.37 -0.07 0.44 0.14 -0.12 -0.02 0.60

4:4 14:15 2:2 5:6 7:8 14:15 11:12 3:4 10:11 14:15 14:15 3:4 5:6 5:6 3:4 1:2 14:15 3:4 3:4 2:2 6:7 14:15 5:6 2:2 6:7 2:2 14:15

8.1E-01 6.8E-01 5.4E-01 7.7E-01 9.5E-02 6.2E-01 5.6E-01 4.9E-01 5.3E-01 9.1E-01 1.9E-03

Page 13 of 26

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116 117 118 119 120 121 122 123 124 125 126 127 128 129 130 131 132 133 134 135 136 137 138 139 140 141 142 143 144 145 146 147 148 149 150 151 152 153 154 155 156 157 158 159 160 161 162 163 164 165 166 167 168 169 170 171 172 173 174 175 176 177 178 179 180 181 182 183 184 185 186 187 188 189 190 191 192 193 194 195 196 197 198 199 200 201 202 203 204 205 206 207 208 209 210 211 212 213 214 215 216 217 218 219 220 221 222 223 224 225 226 227 228 229 230

sp|P27482|CALL3_HUMAN sp|P33908|MA1A1_HUMAN sp|P09211|GSTP1_HUMAN sp|Q08188|TGM3_HUMAN sp|P35321|SPR1A_HUMAN sp|P11021|GRP78_HUMAN sp|P01040|CYTA_HUMAN sp|O43852-4|CALU_HUMAN sp|Q96S21|RB40C_HUMAN sp|P08603|CFAH_HUMAN sp|P12109|CO6A1_HUMAN sp|P01033|TIMP1_HUMAN sp|P63104|1433Z_HUMAN sp|P00558|PGK1_HUMAN sp|Q9UBG3|CRNN_HUMAN sp|P01768|HV307_HUMAN sp|P01703|LV105_HUMAN sp|Q9NZJ4-2|SACS_HUMAN sp|Q9BZ76-2|CNTP3_HUMAN sp|P55058|PLTP_HUMAN sp|P02765|FETUA_HUMAN sp|P02750|A2GL_HUMAN sp|P31947|1433S_HUMAN sp|Q6MZM9|CD040_HUMAN sp|P01859|IGHG2_HUMAN sp|P01621|KV303_HUMAN sp|P01742|HV101_HUMAN sp|P01760|HV105_HUMAN sp|P01778|HV317_HUMAN sp|P01780|HV319_HUMAN sp|P01616|KV203_HUMAN sp|O15084-1|ANR28_HUMAN sp|P01613|KV121_HUMAN sp|Q6UX06|OLFM4_HUMAN sp|P02766|TTHY_HUMAN sp|Q8N4F0|BPIB2_HUMAN sp|P18510-3|IL1RA_HUMAN sp|P13646|K1C13_HUMAN sp|P01767|HV306_HUMAN sp|P02763|A1AG1_HUMAN sp|A8TX70-2|CO6A5_HUMAN sp|Q01469|FABP5_HUMAN sp|P49788|TIG1_HUMAN sp|P58499|FAM3B_HUMAN sp|P02652|APOA2_HUMAN sp|O00584|RNT2_HUMAN sp|P23083|HV103_HUMAN sp|Q15782|CH3L2_HUMAN sp|Q6IE37|OVOS1_HUMAN sp|P11142|HSP7C_HUMAN sp|Q9UBJ2|ABCD2_HUMAN sp|P06331|HV209_HUMAN sp|P00747|PLMN_HUMAN sp|P29508|SPB3_HUMAN sp|Q9HCM4|E41L5_HUMAN sp|Q13023|AKAP6_HUMAN sp|P01773|HV312_HUMAN sp|P60174|TPIS_HUMAN sp|P0C862|C1T9A_HUMAN sp|P54108|CRIS3_HUMAN sp|Q6Q759|SPG17_HUMAN sp|Q8N4C8|MINK1_HUMAN sp|P13647|K2C5_HUMAN sp|P09958|FURIN_HUMAN sp|P15311|EZRI_HUMAN RRRRRsp|Q9Y5G2|PCDGE_HUMAN sp|P27487|DPP4_HUMAN sp|O14802|RPC1_HUMAN RRRRRsp|Q96PV0-4|SYGP1_HUMAN sp|Q14D04|MELT_HUMAN sp|Q9UKX5|ITA11_HUMAN sp|Q8N474|SFRP1_HUMAN sp|P01036|CYTS_HUMAN sp|Q02040|AK17A_HUMAN sp|P07478|TRY2_HUMAN sp|P01700|LV102_HUMAN sp|P01612|KV120_HUMAN sp|Q17RW2|COOA1_HUMAN sp|Q96C34-2|RUND1_HUMAN sp|P12429|ANXA3_HUMAN sp|O14795|UN13B_HUMAN sp|Q14515|SPRL1_HUMAN sp|Q96HE7|ERO1A_HUMAN sp|Q86X29|LSR_HUMAN sp|O00308|WWP2_HUMAN sp|Q5VTE0|EF1A3_HUMAN sp|P04792|HSPB1_HUMAN sp|P02749|APOH_HUMAN sp|P04430|KV122_HUMAN sp|P06316|LV107_HUMAN sp|Q6PJG2|EMSA1_HUMAN sp|Q9C093|SPEF2_HUMAN sp|Q9NQ90|ANO2_HUMAN sp|Q9H0X9|OSBL5_HUMAN sp|Q96L96|ALPK3_HUMAN sp|Q13136|LIPA1_HUMAN sp|B1AJZ9-3|FHAD1_HUMAN sp|P06727|APOA4_HUMAN sp|Q9NQW1|SC31B_HUMAN sp|A2CJ06|DYTN_HUMAN sp|Q96CP6|GRM1A_HUMAN sp|Q9Y6R0|NUMBL_HUMAN sp|P00736|C1R_HUMAN sp|Q14444|CAPR1_HUMAN sp|P29401|TKT_HUMAN sp|Q12791-3|KCMA1_HUMAN sp|Q9P0U4-2|CXXC1_HUMAN sp|O95294|RASL1_HUMAN sp|Q9NR83|S2A4R_HUMAN sp|P07355-2|ANXA2_HUMAN sp|Q5VV42-2|CDKAL_HUMAN sp|Q7L7L0|H2A3_HUMAN sp|Q06830|PRDX1_HUMAN sp|P31151|S10A7_HUMAN sp|P07737|PROF1_HUMAN

Journal of Proteome Research

Calmodulin-like protein 3 OS=Homo sapiens GN=CALML3 PE=1 SV=2 1.2E-01 0.47 Mannosyl-oligosaccharide 1,2-alpha-mannosidase IA OS=Homo sapiens GN=MAN1A1 PE=1 SV=3 2.2E-01 0.69 Glutathione S-transferase P OS=Homo sapiens GN=GSTP1 PE=1 SV=2 7.5E-01 0.73 Protein-glutamine gamma-glutamyltransferase E OS=Homo sapiens GN=TGM3 PE=1 SV=4 1.7E-01 0.53 Cornifin-A OS=Homo sapiens GN=SPRR1A PE=1 SV=2 4.5E-02 0.15 78 kDa glucose-regulated protein OS=Homo sapiens GN=HSPA5 PE=1 SV=2 3.2E-01 0.65 Cystatin-A OS=Homo sapiens GN=CSTA PE=1 SV=1 3.6E-01 0.60 Isoform 4 of Calumenin OS=Homo sapiens GN=CALU 8.1E-01 0.94 Ras-related protein Rab-40C OS=Homo sapiens GN=RAB40C PE=1 SV=1 1.58 Complement factor H OS=Homo sapiens GN=CFH PE=1 SV=4 Collagen alpha-1(VI) chain OS=Homo sapiens GN=COL6A1 PE=1 SV=3 5.5E-01 1.85 Metalloproteinase inhibitor 1 OS=Homo sapiens GN=TIMP1 PE=1 SV=1 9.1E-01 0.97 14-3-3 protein zeta/delta OS=Homo sapiens GN=YWHAZ PE=1 SV=1 5.7E-01 0.67 Phosphoglycerate kinase 1 OS=Homo sapiens GN=PGK1 PE=1 SV=3 3.3E-01 0.69 Cornulin OS=Homo sapiens GN=CRNN PE=1 SV=1 3.2E-01 0.57 Ig heavy chain V-III region CAM OS=Homo sapiens PE=1 SV=1 3.3E-01 6.01 Ig lambda chain V-I region NEWM OS=Homo sapiens PE=1 SV=1 9.5E-01 1.04 Isoform 2 of Sacsin OS=Homo sapiens GN=SACS 8.0E-01 1.09 Isoform 2 of Contactin-associated protein-like 3 OS=Homo sapiens GN=CNTNAP3 6.9E-01 0.94 Phospholipid transfer protein OS=Homo sapiens GN=PLTP PE=1 SV=1 3.8E-01 0.77 Alpha-2-HS-glycoprotein OS=Homo sapiens GN=AHSG PE=1 SV=1 8.9E-01 1.15 Leucine-rich alpha-2-glycoprotein OS=Homo sapiens GN=LRG1 PE=1 SV=2 1.9E-02 0.37 14-3-3 protein sigma OS=Homo sapiens GN=SFN PE=1 SV=1 4.0E-01 0.43 Uncharacterized protein C4orf40 OS=Homo sapiens GN=C4orf40 PE=1 SV=1 3.2E-01 0.61 Ig gamma-2 chain C region OS=Homo sapiens GN=IGHG2 PE=1 SV=2 6.3E-03 3.83 Ig kappa chain V-III region NG9 (Fragment) OS=Homo sapiens PE=1 SV=1 3.2E-01 0.74 Ig heavy chain V-I region EU OS=Homo sapiens PE=1 SV=1 1.6E-01 2.79 Ig heavy chain V-I region WOL OS=Homo sapiens PE=1 SV=1 8.1E-01 1.09 Ig heavy chain V-III region ZAP OS=Homo sapiens PE=1 SV=1 2.7E-01 0.19 Ig heavy chain V-III region JON OS=Homo sapiens PE=1 SV=1 2.0E-02 2.71 Ig kappa chain V-II region MIL OS=Homo sapiens PE=1 SV=1 5.2E-01 0.49 Isoform 3 of Serine/threonine-protein phosphatase 6 regulatory ankyrin repeat subunit A OS=Homo sapiens GN=ANKRD28 Ig kappa chain V-I region Ni OS=Homo sapiens PE=1 SV=1 3.3E-01 0.76 Olfactomedin-4 OS=Homo sapiens GN=OLFM4 PE=1 SV=1 2.9E-01 0.72 Transthyretin OS=Homo sapiens GN=TTR PE=1 SV=1 9.5E-01 0.88 BPI fold-containing family B member 2 OS=Homo sapiens GN=BPIFB2 PE=1 SV=2 2.8E-02 0.30 Isoform 3 of Interleukin-1 receptor antagonist protein OS=Homo sapiens GN=IL1RN 8.3E-02 0.64 Keratin, type I cytoskeletal 13 OS=Homo sapiens GN=KRT13 PE=1 SV=4 8.2E-01 0.66 Ig heavy chain V-III region BUT OS=Homo sapiens PE=1 SV=1 3.0E-01 0.72 Alpha-1-acid glycoprotein 1 OS=Homo sapiens GN=ORM1 PE=1 SV=1 9.9E-01 1.02 Isoform 2 of Collagen alpha-5(VI) chain OS=Homo sapiens GN=COL6A5 7.7E-01 0.86 Fatty acid-binding protein, epidermal OS=Homo sapiens GN=FABP5 PE=1 SV=3 1.2E-01 0.20 Retinoic acid receptor responder protein 1 OS=Homo sapiens GN=RARRES1 PE=2 SV=2 3.5E-01 1.30 Protein FAM3B OS=Homo sapiens GN=FAM3B PE=1 SV=2 8.3E-01 1.04 Apolipoprotein A-II OS=Homo sapiens GN=APOA2 PE=1 SV=1 2.7E-01 5.15 Ribonuclease T2 OS=Homo sapiens GN=RNASET2 PE=1 SV=2 7.7E-01 1.09 Ig heavy chain V-I region V35 OS=Homo sapiens PE=1 SV=1 2.4E-01 1.82 Chitinase-3-like protein 2 OS=Homo sapiens GN=CHI3L2 PE=1 SV=1 9.8E-02 3.96 Ovostatin homolog 1 OS=Homo sapiens GN=OVOS1 PE=2 SV=2 9.2E-01 1.47 Heat shock cognate 71 kDa protein OS=Homo sapiens GN=HSPA8 PE=1 SV=1 5.7E-01 0.68 ATP-binding cassette sub-family D member 2 OS=Homo sapiens GN=ABCD2 PE=1 SV=1 1.6E-01 0.38 Ig heavy chain V-II region ARH-77 OS=Homo sapiens PE=4 SV=1 5.9E-01 1.19 Plasminogen OS=Homo sapiens GN=PLG PE=1 SV=2 1.2E-01 1.36 Serpin B3 OS=Homo sapiens GN=SERPINB3 PE=1 SV=2 2.8E-01 0.38 Band 4.1-like protein 5 OS=Homo sapiens GN=EPB41L5 PE=1 SV=3 A-kinase anchor protein 6 OS=Homo sapiens GN=AKAP6 PE=1 SV=3 Ig heavy chain V-III region BUR OS=Homo sapiens PE=1 SV=1 5.7E-01 1.47 Triosephosphate isomerase OS=Homo sapiens GN=TPI1 PE=1 SV=3 2.7E-01 0.29 Complement C1q and tumor necrosis factor-related protein 9A OS=Homo sapiens GN=C1QTNF9 PE=1 SV=1 Cysteine-rich secretory protein 3 OS=Homo sapiens GN=CRISP3 PE=1 SV=1 2.8E-01 5.65 Sperm-associated antigen 17 OS=Homo sapiens GN=SPAG17 PE=1 SV=1 3.9E-01 0.75 Misshapen-like kinase 1 OS=Homo sapiens GN=MINK1 PE=1 SV=2 Keratin, type II cytoskeletal 5 OS=Homo sapiens GN=KRT5 PE=1 SV=3 5.8E-01 0.66 Furin OS=Homo sapiens GN=FURIN PE=1 SV=2 9.0E-01 1.06 Ezrin OS=Homo sapiens GN=EZR PE=1 SV=4 1.9E-01 0.67 REVERSED Protocadherin gamma-B2 OS=Homo sapiens GN=PCDHGB2 PE=2 SV=1 8.6E-01 1.15 Dipeptidyl peptidase 4 OS=Homo sapiens GN=DPP4 PE=1 SV=2 8.5E-01 1.11 DNA-directed RNA polymerase III subunit RPC1 OS=Homo sapiens GN=POLR3A PE=1 SV=2 REVERSED Isoform 4 of Ras/Rap GTPase-activating protein SynGAP OS=Homo sapiens GN=SYNGAP1 Ventricular zone-expressed PH domain-containing protein homolog 1 OS=Homo sapiens GN=VEPH1 PE=2 SV=1 6.4E-01 0.73 Integrin alpha-11 OS=Homo sapiens GN=ITGA11 PE=1 SV=2 Secreted frizzled-related protein 1 OS=Homo sapiens GN=SFRP1 PE=1 SV=1 4.9E-01 0.83 Cystatin-S OS=Homo sapiens GN=CST4 PE=1 SV=3 2.0E-01 0.27 A-kinase anchor protein 17A OS=Homo sapiens GN=AKAP17A PE=1 SV=2 Trypsin-2 OS=Homo sapiens GN=PRSS2 PE=1 SV=1 1.2E-01 0.76 Ig lambda chain V-I region HA OS=Homo sapiens PE=1 SV=1 3.3E-02 3.65 Ig kappa chain V-I region Mev OS=Homo sapiens PE=1 SV=1 4.4E-01 1.48 Collagen alpha-1(XXIV) chain OS=Homo sapiens GN=COL24A1 PE=2 SV=2 Isoform 2 of RUN domain-containing protein 1 OS=Homo sapiens GN=RUNDC1 Annexin A3 OS=Homo sapiens GN=ANXA3 PE=1 SV=3 3.9E-01 0.38 Protein unc-13 homolog B OS=Homo sapiens GN=UNC13B PE=1 SV=2 SPARC-like protein 1 OS=Homo sapiens GN=SPARCL1 PE=1 SV=2 ERO1-like protein alpha OS=Homo sapiens GN=ERO1L PE=1 SV=2 5.5E-01 0.57 Lipolysis-stimulated lipoprotein receptor OS=Homo sapiens GN=LSR PE=1 SV=4 1.8E-01 0.40 NEDD4-like E3 ubiquitin-protein ligase WWP2 OS=Homo sapiens GN=WWP2 PE=1 SV=2 1.42 Putative elongation factor 1-alpha-like 3 OS=Homo sapiens GN=EEF1A1P5 PE=5 SV=1 Heat shock protein beta-1 OS=Homo sapiens GN=HSPB1 PE=1 SV=2 6.6E-01 0.84 Beta-2-glycoprotein 1 OS=Homo sapiens GN=APOH PE=1 SV=3 1.3E-01 2.02 Ig kappa chain V-I region BAN OS=Homo sapiens PE=1 SV=1 8.7E-01 0.93 Ig lambda chain V-I region BL2 OS=Homo sapiens PE=2 SV=1 2.1E-01 1.63 ELM2 and SANT domain-containing protein 1 OS=Homo sapiens GN=ELMSAN1 PE=1 SV=2 Sperm flagellar protein 2 OS=Homo sapiens GN=SPEF2 PE=1 SV=2 1.9E-01 0.63 Anoctamin-2 OS=Homo sapiens GN=ANO2 PE=1 SV=2 8.3E-02 0.27 Oxysterol-binding protein-related protein 5 OS=Homo sapiens GN=OSBPL5 PE=1 SV=1 2.2E-01 0.73 Alpha-protein kinase 3 OS=Homo sapiens GN=ALPK3 PE=2 SV=2 4.6E-01 4.45 Liprin-alpha-1 OS=Homo sapiens GN=PPFIA1 PE=1 SV=1 Isoform 3 of Forkhead-associated domain-containing protein 1 OS=Homo sapiens GN=FHAD1 8.7E-01 1.06 Apolipoprotein A-IV OS=Homo sapiens GN=APOA4 PE=1 SV=3 9.1E-01 0.91 Protein transport protein Sec31B OS=Homo sapiens GN=SEC31B PE=1 SV=1 7.8E-01 1.14 Dystrotelin OS=Homo sapiens GN=DYTN PE=2 SV=1 GRAM domain-containing protein 1A OS=Homo sapiens GN=GRAMD1A PE=1 SV=2 Numb-like protein OS=Homo sapiens GN=NUMBL PE=1 SV=1 Complement C1r subcomponent OS=Homo sapiens GN=C1R PE=1 SV=2 4.3E-02 2.49 Caprin-1 OS=Homo sapiens GN=CAPRIN1 PE=1 SV=2 Transketolase OS=Homo sapiens GN=TKT PE=1 SV=3 5.4E-01 0.50 Isoform 3 of Calcium-activated potassium channel subunit alpha-1 OS=Homo sapiens GN=KCNMA1 Isoform 2 of CpG-binding protein OS=Homo sapiens GN=CXXC1 RasGAP-activating-like protein 1 OS=Homo sapiens GN=RASAL1 PE=1 SV=3 1.55 SLC2A4 regulator OS=Homo sapiens GN=SLC2A4RG PE=1 SV=4 7.7E-01 1.07 Isoform 2 of Annexin A2 OS=Homo sapiens GN=ANXA2 9.0E-01 0.81 Isoform 2 of Threonylcarbamoyladenosine tRNA methylthiotransferase OS=Homo sapiens GN=CDKAL1 Histone H2A type 3 OS=Homo sapiens GN=HIST3H2A PE=1 SV=3 3.2E-01 4.03 Peroxiredoxin-1 OS=Homo sapiens GN=PRDX1 PE=1 SV=1 9.7E-01 0.98 Protein S100-A7 OS=Homo sapiens GN=S100A7 PE=1 SV=4 8.2E-01 1.10 Profilin-1 OS=Homo sapiens GN=PFN1 PE=1 SV=2 3.2E-01 0.34

-0.33 -0.16 -0.14 -0.28 -0.82 -0.19 -0.22 -0.03 0.20

12:10 13:13 5:4 3:2 7:6 11:10 5:4 4:5 1:3

7.2E-01 4.5E-01 8.9E-01

0.83 0.80 1.19 0.38 0.52 0.66 1.01 2.64 1.03

-0.08 -0.10 0.07 -0.42 -0.29 -0.18 0.01 0.42 0.01

12:9 13:12 5:3 3:1 7:5 11:9 5:3 4:4 1:3

1.8E-01 5.2E-01 7.2E-01

0.27 -0.01 -0.18 -0.16 -0.24 0.78 0.02 0.04 -0.03 -0.12 0.06 -0.44 -0.37 -0.22 0.58 -0.13 0.44 0.04 -0.72 0.43 -0.31

4:4 12:13 5:4 5:4 5:4 5:4 7:6 3:5 2:2 7:6 7:6 7:6 5:4 15:15 15:15 5:4 6:7 10:8 2:2 5:4 9:8

9.3E-01 5.6E-01 3.6E-02 9.4E-01 3.5E-01 9.3E-01 8.8E-01 1.0E-01 1.1E-01 9.1E-01 7.7E-01 1.5E-01 8.5E-01 6.0E-01 1.2E-03 2.0E-01 6.7E-01 2.5E-01 3.9E-01 8.1E-01 4.6E-01

0.93 0.83 4.16 1.03 0.53 0.89 0.92 0.67 0.62 1.04 0.72 0.52 0.79 0.78 6.11 0.63 1.32 1.87 0.25 1.07 0.46

-0.03 -0.08 0.62 0.01 -0.28 -0.05 -0.04 -0.17 -0.21 0.02 -0.14 -0.28 -0.10 -0.11 0.79 -0.20 0.12 0.27 -0.60 0.03 -0.34

-0.12 -0.14 -0.05 -0.52 -0.20 -0.18 -0.14 0.01 -0.07 -0.69 0.11 0.02 0.71 0.04 0.26 0.60 0.17 -0.17 -0.42 0.07 0.13 -0.42

13:13 3:2 2:2 7:6 12:10 3:2 10:8 5:4 2:2 5:4 3:2 7:6 2:2 5:4 13:13 5:4 2:2 5:4 2:2 13:13 2:2 4:4

6.7E-02

0.58 1.73 1.14 0.40 0.74 0.50 0.74 0.44 1.09 0.71 1.31 0.71 2.38 0.71 0.69 5.69 3.48 0.46 0.49 1.17 1.43 0.46

-0.24 0.24 0.06 -0.40 -0.13 -0.30 -0.13 -0.36 0.04 -0.15 0.12 -0.15 0.38 -0.15 -0.16 0.76 0.54 -0.34 -0.31 0.07 0.16 -0.34

1.31 0.50

0.12 3:1 -0.30 3:1

5.0E-01 4.5E-01 9.8E-01 1.4E-01

9.5E-01 1.1E-01 1.5E-01 3.8E-01 5.3E-01 9.0E-01 6.8E-01 1.0E-01 6.5E-01 3.2E-01 4.0E-01 2.7E-02 7.8E-01 4.9E-01 4.8E-01 6.0E-01 1.0E-01 2.9E-01

0.17 3:2 -0.53 3:2

2.3E-01 9.5E-01 3.7E-01 8.2E-02 2.1E-01

0.57 0.87 0.62 1.39 0.29 0.97 0.59 0.35 1.53

-0.25 -0.06 -0.21 0.14 -0.53 -0.01 -0.23 -0.45 0.19

9:10 12:13 3:4 1:2 5:6 9:10 3:4 4:5 3:3

4:4 12:12 5:3 5:3 5:3 5:4 7:5 3:5 2:2 7:5 7:5 7:5 5:3 15:14 15:14 5:3 6:6 10:7 2:2 5:3 9:8

5.3E-01 5.9E-01 6.1E-02 7.2E-02 8.5E-01 3.6E-01 8.1E-01 1.4E-01 1.7E-01 3.6E-01 5.1E-01 3.8E-01 4.9E-01 6.1E-01 4.1E-01 3.4E-01 2.2E-01 3.2E-01 7.0E-01 7.9E-02 9.5E-01

1.98 1.17 0.16 0.67 1.08 6.76 1.13 1.62 1.52 0.73 1.59 0.70 0.54 0.78 0.63 1.18 2.12 0.58 0.75 2.53 1.06

0.30 0.07 -0.79 -0.18 0.03 0.83 0.05 0.21 0.18 -0.13 0.20 -0.15 -0.27 -0.11 -0.20 0.07 0.33 -0.24 -0.12 0.40 0.03

4:4 12:13 3:4 3:4 3:4 4:4 5:6 5:5 2:2 5:6 5:6 5:6 3:4 14:15 14:15 3:4 6:7 7:8 2:2 3:4 8:8

13:12 3:1 2:2 7:5 12:9 3:1 10:7 5:3 2:2 5:3 3:1 7:5 2:2 5:3 13:12 5:3 2:2 5:3 2:2 13:12 2:2 4:4

4.2E-01

1.31 0.41 0.77 0.76 0.86 1.31 0.97 2.32 0.79 0.29 0.99 1.45 2.17 1.53 2.63 0.70 0.42 1.48 0.77 1.01 0.95 0.82

0.12 -0.38 -0.11 -0.12 -0.06 0.12 -0.01 0.36 -0.10 -0.54 -0.01 0.16 0.34 0.18 0.42 -0.16 -0.38 0.17 -0.11 0.01 -0.02 -0.09

12:13 1:2 2:2 5:6 9:10 1:2 7:8 3:4 2:2 3:4 1:2 5:6 2:2 3:4 12:13 3:4 2:2 3:4 2:2 12:13 2:2 4:4

1.12 0.59

0.05 1:2 -0.23 1:2

8.3E-01 6.6E-01 5.7E-01 9.0E-01 5.5E-01 6.0E-01 2.6E-01 1.5E-01 6.0E-01 1.1E-01 5.1E-02 7.0E-01 7.3E-01 7.2E-01 7.6E-01 9.5E-01 6.0E-01 7.2E-01

0.75 2:2 -0.13 3:2

2.4E-01 4.6E-01

2.22 1.29

0.35 2:2 0.11 3:2

5.0E-01 3.4E-02

2.55 0.58

0.41 2:2 -0.24 2:2

-0.18 0.02 -0.17 0.06 0.05

3.6E-01 8.7E-01

-0.38 0.03 -0.22 0.32 -0.44

5:3 8:5 3:1 6:6 8:9

5.5E-01 9.6E-01

4.1E-01 3.8E-02

0.42 1.08 0.60 2.09 0.36

4.6E-01 5.6E-02

1.59 0.97 1.11 0.55 3.06

0.20 -0.01 0.05 -0.26 0.49

5.7E-01

1.48

0.17 4:4

4.0E-01

0.50

-0.30 4:4

5.8E-01 1.4E-01

1.15 6.34

0.06 2:2 0.80 2:2

1.3E-01 1.4E-02

0.72 0.04

-0.14 2:2 -1.37 2:2

2.3E-01 6.2E-01 6.8E-01

0.73 1.13 1.28

-0.13 4:5 0.05 2:2 0.11 7:5

8.5E-01 4.2E-02 7.9E-01

1.04 3.22 1.16

0.02 5:5 0.51 2:2 0.06 5:6

0.47

-0.33 3:1

0.81

-0.09 1:2

5:4 8:6 3:2 6:7 8:9

-0.13 4:4 -0.08 -0.57 2:2 -0.12 4:5 0.56 2:2 0.17 7:6

2:02

-0.42 3:2

3:4 5:6 1:2 6:7 9:9

-0.25 5:4 -0.40 7:6 0.15 1:3

2.1E-01 7.5E-01

3.18 0.71 0.52

0.50 5:3 -0.15 7:5 -0.29 1:3

1.0E-01 5.2E-01 1.7E-01

0.18 0.55 2.75

-0.75 3:4 -0.26 5:6 0.44 3:3

-0.07 0.31 -0.03 0.21

5:4 4:4 12:10 15:15

6.9E-01 7.7E-01 8.1E-01 6.2E-01

0.83 1.19 0.89 0.87

-0.08 0.07 -0.05 -0.06

5:3 4:4 12:9 15:14

9.6E-01 3.2E-01 9.1E-01 9.2E-02

1.01 1.71 1.04 1.87

0.01 0.23 0.02 0.27

3:4 4:4 9:10 14:15

-0.20 -0.57 -0.13 0.65

3:2 3:2 8:6 2:2

3.1E-02 5.6E-02

0.46 0.25 0.57 1.81

-0.34 -0.60 -0.24 0.26

3:1 3:1 8:5 2:2

2.5E-01 6.4E-01

1.39 1.07 1.29 2.45

0.14 0.03 0.11 0.39

1:2 1:2 5:6 2:2

0.02 3:2 -0.04 2:2 0.06 2:2

9.8E-01 4.1E-01 4.0E-01

1.01 0.42 1.53

0.01 3:2 -0.37 2:2 0.18 2:2

9.6E-01 2.2E-01 1.1E-01

1.04 2.15 0.74

0.02 2:2 0.33 2:2 -0.13 2:2

1.69

0.23 3:1

1.47

0.17 1:2

-0.30 5:4

0.40 3:2 9.2E-01

1.10

0.04 5:3

5.2E-01

0.45

-0.35 3:4

0.19 1:3 0.03 3:2 -0.09 4:4

3.38 0.92 0.81

0.53 1:3 -0.04 3:1 -0.09 4:4

6.3E-01

9.0E-01

1.0E+00

0.46 1.16 1.00

-0.34 3:3 0.07 1:2 0.00 4:4

0.61 -0.01 0.04 -0.46

6.3E-01 5.9E-01 4.8E-01 7.6E-01

1.51 1.44 1.37 0.68

0.18 0.16 0.14 -0.17

6.0E-01 5.8E-01 4.8E-01 2.2E-02

2.68 0.68 0.80 0.51

0.43 -0.17 -0.09 -0.30

5:4 5:4 5:4 5:4

ACS Paragon Plus Environment

5:3 5:3 5:3 5:3

3:4 3:4 3:4 3:4

Journal of Proteome Research

1 2 3 Whole Saliva 4 Accession Number and Gene Name 5 Master N 1 sp|Q9HC84|MUC5B_HUMAN 2 sp|P02810|PRPC_HUMAN 6 3 sp|P04745|AMY1_HUMAN 4 sp|P02768|ALBU_HUMAN 7 5 sp|P01833|PIGR_HUMAN 6 sp|P02812|PRB2_HUMAN 8 7 sp|P01876|IGHA1_HUMAN 8 sp|P02788|TRFL_HUMAN 9 9 sp|P60709|ACTB_HUMAN 10 sp|P02538|K2C6A_HUMAN 11 sp|P02814|SMR3B_HUMAN 10 12 sp|P13646|K1C13_HUMAN 13 sp|P01037|CYTN_HUMAN 11 14 sp|Q9UGM3-5|DMBT1_HUMAN 15 sp|P02787|TRFE_HUMAN 12 16 sp|P01834|IGKC_HUMAN 17 sp|P19013|K2C4_HUMAN 13 18 sp|P04406|G3P_HUMAN 19 sp|P25311|ZA2G_HUMAN 14 20 sp|P08779|K1C16_HUMAN 21 sp|P01024|CO3_HUMAN 15 22 sp|P01857|IGHG1_HUMAN 23 sp|P06733|ENOA_HUMAN 16 24 sp|P01591|IGJ_HUMAN 25 sp|P06396|GELS_HUMAN 17 26 sp|Q9UBC9|SPRR3_HUMAN 27 sp|Q04118|PRB3_HUMAN 18 28 sp|P61626|LYSC_HUMAN 29 sp|P22079|PERL_HUMAN 19 30 sp|Q8N4F0|BPIB2_HUMAN 31 sp|P31025|LCN1_HUMAN 20 32 sp|P04083|ANXA1_HUMAN 33 sp|A8K2U0|A2ML1_HUMAN 21 34 sp|P08107|HSP71_HUMAN 35 sp|B9A064|IGLL5_HUMAN 36 sp|P04264|K2C1_HUMAN 22 37 sp|P13647|K2C5_HUMAN 38 sp|P12273|PIP_HUMAN 23 39 sp|P05164|PERM_HUMAN 40 sp|Q9Y6R7|FCGBP_HUMAN 24 41 sp|P00738|HPT_HUMAN 42 sp|P01877|IGHA2_HUMAN 25 43 sp|Q01469|FABP5_HUMAN 44 sp|P07237|PDIA1_HUMAN 26 45 sp|P01871|IGHM_HUMAN 46 sp|P13796|PLSL_HUMAN 27 47 sp|P04080|CYTB_HUMAN 48 sp|P14618|KPYM_HUMAN 28 49 sp|Q9UBG3|CRNN_HUMAN 50 sp|P18136|KV313_HUMAN 29 51 sp|P15515|HIS1_HUMAN 52 sp|P01036|CYTS_HUMAN 30 53 sp|Q96DR5|BPIA2_HUMAN 54 sp|P02647|APOA1_HUMAN 31 55 sp|P01609|KV117_HUMAN 56 sp|Q8TDL5|BPIB1_HUMAN 32 57 sp|P00558|PGK1_HUMAN 58 sp|P63104|1433Z_HUMAN 33 60 sp|P06702|S10A9_HUMAN 61 sp|P01023|A2MG_HUMAN 62 sp|P09211|GSTP1_HUMAN 34 63 sp|P06753-3|TPM3_HUMAN 64 sp|P04075-2|ALDOA_HUMAN 35 65 sp|P07737|PROF1_HUMAN 66 sp|P29401|TKT_HUMAN 36 67 sp|P23280-2|CAH6_HUMAN 68 sp|P54108|CRIS3_HUMAN 37 69 sp|Q6P5S2|CF058_HUMAN 70 sp|P60174|TPIS_HUMAN 38 71 sp|P15311|EZRI_HUMAN 72 sp|P05109|S10A8_HUMAN 39 73 sp|P13645|K1C10_HUMAN 74 sp|P62937|PPIA_HUMAN 40 75 sp|P14780|MMP9_HUMAN 76 sp|P02533|K1C14_HUMAN 41 77 sp|P16403|H12_HUMAN 78 sp|Q6UWP8|SBSN_HUMAN 42 79 sp|P32926|DSG3_HUMAN 80 sp|P02671|FIBA_HUMAN 43 81 sp|P52209|6PGD_HUMAN 82 sp|Q5QNW6|H2B2F_HUMAN 44 83 sp|Q96DA0|ZG16B_HUMAN 84 sp|P26038|MOES_HUMAN 45 85 sp|P06744-2|G6PI_HUMAN 86 sp|P37837|TALDO_HUMAN 87 sp|P31947|1433S_HUMAN 46 88 sp|P01766|HV305_HUMAN 89 sp|Q9NQ38|ISK5_HUMAN 47 90 sp|P31146|COR1A_HUMAN 91 sp|Q8TAX7|MUC7_HUMAN 48 92 sp|P30740|ILEU_HUMAN 93 sp|P02774-3|VTDB_HUMAN 49 94 sp|P10909-2|CLUS_HUMAN 95 sp|P35527|K1C9_HUMAN 50 96 sp|Q01546|K22O_HUMAN 97 sp|Q02487|DSC2_HUMAN 51 98 sp|P01034|CYTC_HUMAN 99 sp|P18510-2|IL1RA_HUMAN 52 100 sp|P09228|CYTT_HUMAN 101 sp|Q07654-2|TFF3_HUMAN 53 102 sp|O95274|LYPD3_HUMAN 103 sp|P06309|KV205_HUMAN 54 104 sp|P00338|LDHA_HUMAN 105 sp|P03973|SLPI_HUMAN 55 106 sp|P01859|IGHG2_HUMAN 107 sp|Q08380|LG3BP_HUMAN 56 108 sp|P04433|KV309_HUMAN 109 sp|P01611|KV119_HUMAN 57 110 sp|P02675|FIBB_HUMAN 111 sp|P09960|LKHA4_HUMAN 112 sp|P11021|GRP78_HUMAN 58 113 sp|P78385|KRT83_HUMAN 114 sp|P80188|NGAL_HUMAN 59 115 sp|P62805|H4_HUMAN 60

Protein Name Mucin-5B OS=Homo sapiens GN=MUC5B PE=1 SV=3 Salivary acidic proline-rich phosphoprotein 1/2 OS=Homo sapiens GN=PRH1 PE=1 SV=2 Alpha-amylase 1 OS=Homo sapiens GN=AMY1A PE=1 SV=2 Serum albumin OS=Homo sapiens GN=ALB PE=1 SV=2 Polymeric immunoglobulin receptor OS=Homo sapiens GN=PIGR PE=1 SV=4 Basic salivary proline-rich protein 2 OS=Homo sapiens GN=PRB2 PE=1 SV=3 Ig alpha-1 chain C region OS=Homo sapiens GN=IGHA1 PE=1 SV=2 Lactotransferrin OS=Homo sapiens GN=LTF PE=1 SV=6 Actin, cytoplasmic 1 OS=Homo sapiens GN=ACTB PE=1 SV=1 Keratin, type II cytoskeletal 6A OS=Homo sapiens GN=KRT6A PE=1 SV=3 Submaxillary gland androgen-regulated protein 3B OS=Homo sapiens GN=SMR3B PE=1 SV=2 Keratin, type I cytoskeletal 13 OS=Homo sapiens GN=KRT13 PE=1 SV=4 Cystatin-SN OS=Homo sapiens GN=CST1 PE=1 SV=3 Isoform 5 of Deleted in malignant brain tumors 1 protein OS=Homo sapiens GN=DMBT1 Serotransferrin OS=Homo sapiens GN=TF PE=1 SV=3 Ig kappa chain C region OS=Homo sapiens GN=IGKC PE=1 SV=1 Keratin, type II cytoskeletal 4 OS=Homo sapiens GN=KRT4 PE=1 SV=4 Glyceraldehyde-3-phosphate dehydrogenase OS=Homo sapiens GN=GAPDH PE=1 SV=3 Zinc-alpha-2-glycoprotein OS=Homo sapiens GN=AZGP1 PE=1 SV=2 Keratin, type I cytoskeletal 16 OS=Homo sapiens GN=KRT16 PE=1 SV=4 Complement C3 OS=Homo sapiens GN=C3 PE=1 SV=2 Ig gamma-1 chain C region OS=Homo sapiens GN=IGHG1 PE=1 SV=1 Alpha-enolase OS=Homo sapiens GN=ENO1 PE=1 SV=2 Immunoglobulin J chain OS=Homo sapiens GN=IGJ PE=1 SV=4 Gelsolin OS=Homo sapiens GN=GSN PE=1 SV=1 Small proline-rich protein 3 OS=Homo sapiens GN=SPRR3 PE=1 SV=2 Basic salivary proline-rich protein 3 OS=Homo sapiens GN=PRB3 PE=1 SV=2 Lysozyme C OS=Homo sapiens GN=LYZ PE=1 SV=1 Lactoperoxidase OS=Homo sapiens GN=LPO PE=1 SV=2 BPI fold-containing family B member 2 OS=Homo sapiens GN=BPIFB2 PE=1 SV=2 Lipocalin-1 OS=Homo sapiens GN=LCN1 PE=1 SV=1 Annexin A1 OS=Homo sapiens GN=ANXA1 PE=1 SV=2 Alpha-2-macroglobulin-like protein 1 OS=Homo sapiens GN=A2ML1 PE=1 SV=3 Heat shock 70 kDa protein 1A/1B OS=Homo sapiens GN=HSPA1A PE=1 SV=5 Immunoglobulin lambda-like polypeptide 5 OS=Homo sapiens GN=IGLL5 PE=2 SV=2 Keratin, type II cytoskeletal 1 OS=Homo sapiens GN=KRT1 PE=1 SV=6 Keratin, type II cytoskeletal 5 OS=Homo sapiens GN=KRT5 PE=1 SV=3 Prolactin-inducible protein OS=Homo sapiens GN=PIP PE=1 SV=1 Myeloperoxidase OS=Homo sapiens GN=MPO PE=1 SV=1 IgGFc-binding protein OS=Homo sapiens GN=FCGBP PE=1 SV=3 Haptoglobin OS=Homo sapiens GN=HP PE=1 SV=1 Ig alpha-2 chain C region OS=Homo sapiens GN=IGHA2 PE=1 SV=3 Fatty acid-binding protein, epidermal OS=Homo sapiens GN=FABP5 PE=1 SV=3 Protein disulfide-isomerase OS=Homo sapiens GN=P4HB PE=1 SV=3 Ig mu chain C region OS=Homo sapiens GN=IGHM PE=1 SV=3 Plastin-2 OS=Homo sapiens GN=LCP1 PE=1 SV=6 Cystatin-B OS=Homo sapiens GN=CSTB PE=1 SV=2 Pyruvate kinase PKM OS=Homo sapiens GN=PKM PE=1 SV=4 Cornulin OS=Homo sapiens GN=CRNN PE=1 SV=1 Ig kappa chain V-III region HIC OS=Homo sapiens PE=2 SV=2 Histatin-1 OS=Homo sapiens GN=HTN1 PE=1 SV=2 Cystatin-S OS=Homo sapiens GN=CST4 PE=1 SV=3 BPI fold-containing family A member 2 OS=Homo sapiens GN=BPIFA2 PE=1 SV=2 Apolipoprotein A-I OS=Homo sapiens GN=APOA1 PE=1 SV=1 Ig kappa chain V-I region Scw OS=Homo sapiens PE=1 SV=1 BPI fold-containing family B member 1 OS=Homo sapiens GN=BPIFB1 PE=2 SV=1 Phosphoglycerate kinase 1 OS=Homo sapiens GN=PGK1 PE=1 SV=3 14-3-3 protein zeta/delta OS=Homo sapiens GN=YWHAZ PE=1 SV=1 Protein S100-A9 OS=Homo sapiens GN=S100A9 PE=1 SV=1 Alpha-2-macroglobulin OS=Homo sapiens GN=A2M PE=1 SV=3 Glutathione S-transferase P OS=Homo sapiens GN=GSTP1 PE=1 SV=2 Isoform 3 of Tropomyosin alpha-3 chain OS=Homo sapiens GN=TPM3 Isoform 2 of Fructose-bisphosphate aldolase A OS=Homo sapiens GN=ALDOA Profilin-1 OS=Homo sapiens GN=PFN1 PE=1 SV=2 Transketolase OS=Homo sapiens GN=TKT PE=1 SV=3 Isoform 2 of Carbonic anhydrase 6 OS=Homo sapiens GN=CA6 Cysteine-rich secretory protein 3 OS=Homo sapiens GN=CRISP3 PE=1 SV=1 UPF0762 protein C6orf58 OS=Homo sapiens GN=C6orf58 PE=1 SV=2 Triosephosphate isomerase OS=Homo sapiens GN=TPI1 PE=1 SV=3 Ezrin OS=Homo sapiens GN=EZR PE=1 SV=4 Protein S100-A8 OS=Homo sapiens GN=S100A8 PE=1 SV=1 Keratin, type I cytoskeletal 10 OS=Homo sapiens GN=KRT10 PE=1 SV=6 Peptidyl-prolyl cis-trans isomerase A OS=Homo sapiens GN=PPIA PE=1 SV=2 Matrix metalloproteinase-9 OS=Homo sapiens GN=MMP9 PE=1 SV=3 Keratin, type I cytoskeletal 14 OS=Homo sapiens GN=KRT14 PE=1 SV=4 Histone H1.2 OS=Homo sapiens GN=HIST1H1C PE=1 SV=2 Suprabasin OS=Homo sapiens GN=SBSN PE=2 SV=2 Desmoglein-3 OS=Homo sapiens GN=DSG3 PE=1 SV=2 Fibrinogen alpha chain OS=Homo sapiens GN=FGA PE=1 SV=2 6-phosphogluconate dehydrogenase, decarboxylating OS=Homo sapiens GN=PGD PE=1 SV=3 Histone H2B type 2-F OS=Homo sapiens GN=HIST2H2BF PE=1 SV=3 Zymogen granule protein 16 homolog B OS=Homo sapiens GN=ZG16B PE=1 SV=3 Moesin OS=Homo sapiens GN=MSN PE=1 SV=3 Isoform 2 of Glucose-6-phosphate isomerase OS=Homo sapiens GN=GPI Transaldolase OS=Homo sapiens GN=TALDO1 PE=1 SV=2 14-3-3 protein sigma OS=Homo sapiens GN=SFN PE=1 SV=1 Ig heavy chain V-III region BRO OS=Homo sapiens PE=1 SV=1 Serine protease inhibitor Kazal-type 5 OS=Homo sapiens GN=SPINK5 PE=1 SV=2 Coronin-1A OS=Homo sapiens GN=CORO1A PE=1 SV=4 Mucin-7 OS=Homo sapiens GN=MUC7 PE=1 SV=2 Leukocyte elastase inhibitor OS=Homo sapiens GN=SERPINB1 PE=1 SV=1 Isoform 3 of Vitamin D-binding protein OS=Homo sapiens GN=GC Isoform 2 of Clusterin OS=Homo sapiens GN=CLU Keratin, type I cytoskeletal 9 OS=Homo sapiens GN=KRT9 PE=1 SV=3 Keratin, type II cytoskeletal 2 oral OS=Homo sapiens GN=KRT76 PE=1 SV=2 Desmocollin-2 OS=Homo sapiens GN=DSC2 PE=1 SV=1 Cystatin-C OS=Homo sapiens GN=CST3 PE=1 SV=1 Isoform 2 of Interleukin-1 receptor antagonist protein OS=Homo sapiens GN=IL1RN Cystatin-SA OS=Homo sapiens GN=CST2 PE=1 SV=1 Isoform 2 of Trefoil factor 3 OS=Homo sapiens GN=TFF3 Ly6/PLAUR domain-containing protein 3 OS=Homo sapiens GN=LYPD3 PE=1 SV=2 Ig kappa chain V-II region GM607 (Fragment) OS=Homo sapiens PE=4 SV=1 L-lactate dehydrogenase A chain OS=Homo sapiens GN=LDHA PE=1 SV=2 Antileukoproteinase OS=Homo sapiens GN=SLPI PE=1 SV=2 Ig gamma-2 chain C region OS=Homo sapiens GN=IGHG2 PE=1 SV=2 Galectin-3-binding protein OS=Homo sapiens GN=LGALS3BP PE=1 SV=1 Ig kappa chain V-III region VG (Fragment) OS=Homo sapiens PE=1 SV=1 Ig kappa chain V-I region Wes OS=Homo sapiens PE=1 SV=1 Fibrinogen beta chain OS=Homo sapiens GN=FGB PE=1 SV=2 Leukotriene A-4 hydrolase OS=Homo sapiens GN=LTA4H PE=1 SV=2 78 kDa glucose-regulated protein OS=Homo sapiens GN=HSPA5 PE=1 SV=2 Keratin, type II cuticular Hb3 OS=Homo sapiens GN=KRT83 PE=1 SV=2 Neutrophil gelatinase-associated lipocalin OS=Homo sapiens GN=LCN2 PE=1 SV=2 Histone H4 OS=Homo sapiens GN=HIST1H4A PE=1 SV=2

Page 14 of 26

pSS / HC pSS / HC pSS / HC pSS / HC pSS / SC pSS / SC pSS / SC pSS / SC SC / HC ttest fold lin fold log n1-n2 ttest fold lin fold log n1-n2 ttest 1.3E-05 2.5E-02 1.1E-02 1.6E-01 3.6E-01 4.3E-01 6.4E-02 3.9E-01 1.6E-01 2.1E-02 3.7E-01 4.0E-03 8.4E-02 1.4E-02 7.4E-01 1.8E-02 4.0E-01 7.0E-02 3.9E-01 6.2E-02 6.0E-01 3.2E-02 6.6E-01 3.8E-02 9.7E-01 2.9E-01 5.1E-01 2.9E-01 9.3E-02 2.9E-05 1.4E-03 1.1E-02 9.3E-01 5.4E-01 1.2E-02 7.9E-01 1.2E-01 3.0E-02 1.3E-01 5.1E-01 9.7E-01 4.6E-02 8.8E-01 9.6E-01 6.1E-01 7.3E-01 9.9E-01 2.2E-01 4.1E-02 1.4E-02 4.5E-03 7.2E-02 7.7E-04 8.3E-01 1.3E-01 1.2E-05 2.4E-01 3.5E-03 3.6E-01 4.9E-01 1.5E-01 9.7E-01 1.3E-01 5.9E-01 1.5E-01 1.1E-03 3.0E-02 1.1E-01 6.7E-01 9.8E-01 7.4E-02 6.8E-01 3.0E-01 4.3E-01 2.0E-01 2.3E-01 3.8E-01 9.3E-01 5.7E-01 6.1E-03 6.3E-04 4.9E-01 9.0E-01 5.8E-01 7.9E-01 9.7E-01 9.8E-01 4.3E-01 5.3E-01 2.5E-01 2.6E-01 9.1E-02 9.3E-01 1.7E-01 2.2E-01 1.5E-01 5.1E-02 1.0E-01 1.6E-02 5.5E-02 6.6E-01 5.0E-01 6.2E-01 6.8E-01 7.8E-01 3.0E-01 3.5E-01 8.9E-01 4.1E-02 4.3E-01 7.2E-01 7.8E-01 2.9E-01 1.1E-02

0.12 0.08 0.27 0.61 1.55 0.42 2.42 1.51 0.58 3.99 0.35 5.38 0.22 0.36 1.12 2.53 3.08 0.65 0.66 5.30 0.84 2.84 1.19 2.19 0.99 0.56 0.56 0.51 0.44 0.10 0.22 3.67 0.96 0.81 2.97 0.84 4.58 0.32 2.27 1.65 0.99 0.34 0.93 0.97 1.27 0.88 1.00 0.58 0.41 2.44 0.16 0.15 0.11 1.10 2.85 0.07 0.58 0.40 1.81 0.70 0.58 0.98 0.55 0.64 0.51 0.13 0.43 0.49 0.87 1.01 3.20 1.18 0.68 1.45 3.66 1.70 1.67 0.93 0.83 0.37 6.76 0.72 1.07 0.82 0.93 1.03 1.02 1.42 1.24 0.36 0.76 1.88 1.05 0.41 5.04 1.79 0.31 0.41 0.27 0.39 1.24 1.28 0.88 0.79 0.90 1.38 1.33 1.14 0.65 1.40 0.95 2.08 1.86 9.26

-0.92 -1.07 -0.56 -0.21 0.19 -0.38 0.38 0.18 -0.23 0.60 -0.46 0.73 -0.66 -0.44 0.05 0.40 0.49 -0.19 -0.18 0.72 -0.07 0.45 0.08 0.34 -0.01 -0.25 -0.25 -0.29 -0.36 -1.02 -0.66 0.57 -0.02 -0.09 0.47 -0.07 0.66 -0.50 0.36 0.22 -0.01 -0.47 -0.03 -0.01 0.11 -0.05 0.00 -0.23 -0.39 0.39 -0.79 -0.81 -0.95 0.04 0.45 -1.15 -0.23 -0.40 0.26 -0.15 -0.23 -0.01 -0.26 -0.19 -0.29 -0.89 -0.37 -0.31 -0.06 0.00 0.51 0.07 -0.17 0.16 0.56 0.23 0.22 -0.03 -0.08 -0.43 0.83 -0.14 0.03 -0.09 -0.03 0.01 0.01 0.15 0.09 -0.45 -0.12 0.27 0.02 -0.39 0.70 0.25 -0.51 -0.39 -0.57 -0.41 0.09 0.11 -0.06 -0.10 -0.05 0.14 0.13 0.06 -0.19 0.14 -0.02 0.32 0.27 0.97

15:15 3:3 15:15 15:15 15:15 3:3 15:15 15:15 13:13 11:11 5:5 13:13 9:9 15:15 15:15 15:15 5:5 13:13 15:15 6:6 15:15 13:13 13:13 15:15 13:13 13:13 2:2 15:15 13:13 11:11 15:15 11:11 13:13 15:15 9:9 11:11 4:4 15:15 13:13 10:10 13:13 11:11 13:13 11:11 15:15 11:11 13:13 13:13 13:13 13:13 15:15 4:4 15:15 13:13 6:6 11:11 11:11 15:15 13:13 13:13 7:7 11:11 11:11 9:9 11:11 11:11 15:15 15:15 15:15 13:13 13:13 9:9 11:11 11:11 5:5 5:5 9:9 11:11 13:13 11:11 13:13 15:15 13:13 15:15 13:13 5:5 13:13 7:7 13:13 11:11 11:11 7:7 9:9 8:8 2:2 15:15 11:11 9:9 9:9 9:9 15:15 13:13 15:15 13:13 13:13 13:13 10:10 9:9 11:11 5:5 3:3 2:2 9:9 3:3

ACS Paragon Plus Environment

2.4E-01 1.1E-02 3.5E-02 3.3E-01 5.8E-01 3.0E-01 6.0E-01 4.2E-02 9.6E-01 2.1E-01 1.5E-02 5.9E-01 8.8E-02 9.7E-03 1.2E-01 2.4E-01 9.9E-01 1.1E-01 1.5E-01 5.6E-01 9.6E-01 1.2E-02 5.6E-01 5.8E-01 7.2E-01 7.3E-01 7.4E-01 9.3E-01 1.5E-01 2.6E-01 2.9E-01 2.1E-01 8.8E-01 9.1E-01 1.5E-01 6.6E-01 6.3E-01 1.7E-01 3.5E-02 6.9E-01 1.9E-01 5.3E-03 4.4E-01 7.5E-01 6.6E-01 9.1E-01 7.0E-01 1.9E-01 4.1E-01 5.4E-02 5.2E-04 8.8E-02 3.4E-03 7.7E-01 5.8E-01 6.1E-01 9.3E-01 8.7E-01 3.7E-01 5.1E-01 4.8E-01 8.4E-01 6.1E-01 9.9E-01 3.0E-01 4.8E-04 4.3E-02 2.7E-02 8.0E-01 7.6E-01 1.7E-01 5.8E-01 8.5E-01 7.7E-01 4.9E-01 8.9E-01 9.5E-01 7.0E-01 5.9E-01 6.6E-01 8.2E-02 8.5E-01 9.6E-01 6.3E-01 6.4E-01 5.4E-01 7.0E-01 2.6E-01 2.6E-02 1.7E-01 7.9E-01 3.0E-01 1.9E-01 3.8E-01 1.9E-01 9.1E-01 3.5E-01 4.9E-01 9.3E-02 9.8E-01 7.5E-01 9.7E-01 9.6E-01 8.1E-01 6.1E-01 9.2E-02 4.2E-01 8.2E-01 5.8E-01 1.6E-01 1.4E-01 5.7E-01 7.8E-01 2.4E-02

1.68 0.03 0.36 1.50 0.77 0.20 1.25 2.77 1.02 2.25 0.05 1.37 0.20 0.34 1.82 1.59 0.98 1.61 0.51 1.57 1.02 3.29 1.27 1.22 0.86 0.81 0.65 0.95 0.50 0.60 1.74 1.69 1.07 0.96 1.88 1.39 1.52 0.44 3.41 1.32 1.61 0.23 1.57 1.10 1.20 1.04 1.27 2.11 0.69 1.94 0.12 0.25 0.14 1.12 1.43 1.26 1.05 0.95 1.77 1.39 1.45 1.15 0.79 1.01 0.61 0.13 0.44 0.38 0.91 1.12 2.51 1.27 1.10 1.19 1.86 0.94 1.04 1.47 1.26 0.83 2.72 0.90 0.98 1.30 1.16 2.11 0.79 1.58 2.01 0.29 0.94 1.74 2.31 0.61 2.95 1.03 0.51 0.65 0.31 1.02 1.17 0.99 0.99 1.14 1.29 1.66 1.34 1.23 0.89 2.20 1.22 5.37 1.19 6.73

0.22 -1.59 -0.44 0.18 -0.12 -0.70 0.10 0.44 0.01 0.35 -1.30 0.14 -0.70 -0.47 0.26 0.20 -0.01 0.21 -0.29 0.20 0.01 0.52 0.10 0.08 -0.07 -0.09 -0.19 -0.02 -0.30 -0.23 0.24 0.23 0.03 -0.02 0.27 0.14 0.18 -0.36 0.53 0.12 0.21 -0.64 0.20 0.04 0.08 0.02 0.10 0.32 -0.16 0.29 -0.93 -0.61 -0.85 0.05 0.15 0.10 0.02 -0.02 0.25 0.14 0.16 0.06 -0.10 0.00 -0.22 -0.88 -0.35 -0.42 -0.04 0.05 0.40 0.10 0.04 0.08 0.27 -0.03 0.02 0.17 0.10 -0.08 0.44 -0.05 -0.01 0.11 0.06 0.32 -0.10 0.20 0.30 -0.54 -0.03 0.24 0.36 -0.21 0.47 0.01 -0.29 -0.18 -0.50 0.01 0.07 -0.01 -0.01 0.06 0.11 0.22 0.13 0.09 -0.05 0.34 0.09 0.73 0.07 0.83

15:15 3:3 15:15 15:15 15:15 3:3 15:15 15:15 13:13 11:11 5:5 13:13 9:9 15:15 15:15 15:15 5:5 13:13 15:15 6:6 15:15 13:13 13:13 15:15 13:13 13:13 2:2 15:15 13:13 11:11 15:15 11:11 13:13 15:15 9:9 11:11 4:4 15:15 13:13 10:10 13:13 11:11 13:13 11:11 15:15 11:11 13:13 13:13 13:13 13:13 15:15 4:4 15:15 13:13 6:6 11:11 11:11 15:15 13:13 13:13 7:7 11:11 11:11 9:9 11:11 11:11 15:15 15:15 15:15 13:13 13:13 9:9 11:11 11:11 5:5 5:5 9:9 11:11 13:13 11:11 13:13 15:15 13:13 15:15 13:13 5:5 13:13 7:7 13:13 11:11 11:11 7:7 9:9 8:8 2:2 15:15 11:11 9:9 9:9 9:9 15:15 13:13 15:15 13:13 13:13 13:13 10:10 9:9 11:11 5:5 3:3 2:2 9:9 3:3

5.3E-09 3.1E-01 3.8E-01 1.3E-02 1.0E-01 6.3E-01 1.1E-01 2.1E-01 1.3E-01 3.5E-01 3.1E-02 1.2E-02 9.0E-01 7.9E-01 2.0E-01 2.9E-01 1.5E-01 2.5E-03 4.4E-01 2.1E-01 5.8E-01 7.7E-01 8.8E-01 7.5E-02 7.3E-01 5.1E-01 8.8E-01 2.6E-01 6.6E-01 2.6E-05 1.2E-04 2.7E-02 8.4E-01 5.8E-01 4.1E-01 4.9E-01 1.8E-01 4.7E-01 5.4E-01 7.7E-01 1.1E-01 2.3E-01 4.2E-01 8.2E-01 8.8E-01 5.9E-01 7.3E-01 5.8E-03 1.6E-01 4.3E-01 5.6E-01 5.5E-01 6.5E-01 9.5E-01 2.9E-01 4.2E-06 3.0E-01 2.5E-03 9.7E-01 1.4E-01 9.2E-02 8.0E-01 3.2E-01 5.9E-01 6.5E-01 9.3E-01 8.8E-01 5.2E-01 8.7E-01 7.8E-01 7.1E-01 8.8E-01 1.8E-01 6.9E-01 5.2E-01 1.4E-01 2.8E-01 6.3E-01 2.8E-01 1.3E-02 1.3E-01 6.4E-01 8.1E-01 3.3E-01 5.1E-01 5.4E-01 6.7E-01 8.0E-01 8.3E-02 7.6E-01 3.1E-01 8.8E-01 1.9E-01 3.5E-01 5.5E-01 1.5E-01 3.0E-01 4.3E-01 7.8E-01 6.1E-02 8.9E-01 5.2E-01 6.6E-01 4.6E-01 4.4E-01 5.4E-01 9.8E-01 9.4E-01 2.0E-01 4.8E-01 1.7E-01 4.9E-01 3.7E-01 4.3E-01

SC / HC fold lin 0.07 3.26 0.76 0.41 2.02 2.07 1.94 0.55 0.57 1.78 6.92 3.94 1.10 1.07 0.62 1.59 3.14 0.40 1.29 3.38 0.83 0.86 0.94 1.80 1.15 0.69 0.86 0.54 0.88 0.16 0.13 2.18 0.90 0.85 1.58 0.61 3.01 0.71 0.67 1.25 0.61 1.48 0.59 0.89 1.06 0.85 0.79 0.28 0.60 1.26 1.36 0.63 0.80 0.97 2.00 0.06 0.56 0.42 1.02 0.51 0.40 0.85 0.69 0.64 0.85 0.97 0.97 1.27 0.95 0.90 1.28 0.93 0.62 1.22 1.97 1.82 1.61 0.64 0.65 0.44 2.48 0.80 1.09 0.63 0.80 0.49 1.29 0.89 0.62 1.24 0.81 1.08 0.46 0.67 1.71 1.73 0.61 0.63 0.85 0.38 1.06 1.30 0.89 0.69 0.70 0.83 0.99 0.93 0.73 0.64 0.78 0.39 1.57 1.38

SC / HC SC / HC fold log n1-n2 -1.15 0.51 -0.12 -0.39 0.31 0.32 0.29 -0.26 -0.24 0.25 0.84 0.60 0.04 0.03 -0.21 0.20 0.50 -0.39 0.11 0.53 -0.08 -0.06 -0.03 0.25 0.06 -0.16 -0.06 -0.27 -0.06 -0.80 -0.90 0.34 -0.05 -0.07 0.20 -0.22 0.48 -0.15 -0.18 0.10 -0.21 0.17 -0.23 -0.05 0.03 -0.07 -0.10 -0.56 -0.22 0.10 0.13 -0.20 -0.10 -0.01 0.30 -1.25 -0.26 -0.37 0.01 -0.29 -0.40 -0.07 -0.16 -0.19 -0.07 -0.01 -0.01 0.11 -0.02 -0.04 0.11 -0.03 -0.21 0.08 0.29 0.26 0.21 -0.20 -0.18 -0.35 0.39 -0.10 0.04 -0.20 -0.10 -0.31 0.11 -0.05 -0.21 0.09 -0.09 0.03 -0.34 -0.17 0.23 0.24 -0.22 -0.20 -0.07 -0.42 0.03 0.11 -0.05 -0.16 -0.16 -0.08 0.00 -0.03 -0.14 -0.20 -0.11 -0.41 0.19 0.14

15:15 3:3 15:15 15:15 15:15 3:3 15:15 15:15 13:13 11:11 5:5 13:13 9:9 15:15 15:15 15:15 5:5 13:13 15:15 6:6 15:15 13:13 13:13 15:15 13:13 13:13 2:2 15:15 13:13 11:11 15:15 11:11 13:13 15:15 9:9 11:11 4:4 15:15 13:13 10:10 13:13 11:11 13:13 11:11 15:15 11:11 13:13 13:13 13:13 13:13 15:15 4:4 15:15 13:13 6:6 11:11 11:11 15:15 13:13 13:13 7:7 11:11 11:11 9:9 11:11 11:11 15:15 15:15 15:15 13:13 13:13 9:9 11:11 11:11 5:5 5:5 9:9 11:11 13:13 11:11 13:13 15:15 13:13 15:15 13:13 5:5 13:13 7:7 13:13 11:11 11:11 7:7 9:9 8:8 2:2 15:15 11:11 9:9 9:9 9:9 15:15 13:13 15:15 13:13 13:13 13:13 10:10 9:9 11:11 5:5 3:3 2:2 9:9 3:3

Page 15 of 26

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 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 60

116 117 118 119 120 121 122 123 124 125 126 127 128 129 130 131 132 133 134 135 136 137 138 139 140 141 142 143 144 145 147 148 150 151 152 153 154 155 156 157 158 159 160 161 162 164 165 166 167 168 169 170 171 172 173 174 175 176 177 178 179 180 181 182 183 184 185 186 187 188 189 190 192 193 194 195 196 197 198 199 200 201 202 203 204 205 206 207 208 209 210 211 212 213 214 215 216 217 218 219 220 221 222 223 224 225 226 228 230 231 233 234 235 237 238 240 241 243 244 246 247 248

sp|P01009|A1AT_HUMAN sp|P27482|CALL3_HUMAN sp|Q02413|DSG1_HUMAN sp|Q71DI3|H32_HUMAN sp|P62328|TYB4_HUMAN sp|P80748|LV302_HUMAN sp|P08311|CATG_HUMAN sp|P04792|HSPB1_HUMAN sp|P10599|THIO_HUMAN sp|P52566|GDIR2_HUMAN sp|P06870|KLK1_HUMAN sp|Q06830|PRDX1_HUMAN sp|P11142|HSP7C_HUMAN sp|Q08188|TGM3_HUMAN sp|Q01518|CAP1_HUMAN sp|Q14508|WFDC2_HUMAN sp|P20061|TCO1_HUMAN sp|P01040|CYTA_HUMAN sp|P28325|CYTD_HUMAN sp|P29508|SPB3_HUMAN sp|P35321|SPR1A_HUMAN sp|P04040|CATA_HUMAN sp|P07355|ANXA2_HUMAN sp|P0CG05|LAC2_HUMAN sp|P23284|PPIB_HUMAN sp|P02765|FETUA_HUMAN sp|P80303|NUCB2_HUMAN sp|P02652|APOA2_HUMAN sp|P59666|DEF3_HUMAN sp|P25815|S100P_HUMAN sp|P01714|LV301_HUMAN sp|P01624|KV306_HUMAN sp|P01598|KV106_HUMAN sp|P35908|K22E_HUMAN sp|P06314|KV404_HUMAN sp|P69905|HBA_HUMAN sp|P01764|HV303_HUMAN sp|P23528|COF1_HUMAN sp|P05204|HMGN2_HUMAN sp|Q04695|K1C17_HUMAN sp|P18206|VINC_HUMAN sp|P80723|BASP1_HUMAN sp|P35579|MYH9_HUMAN sp|Q8NBJ4|GOLM1_HUMAN sp|P08123|CO1A2_HUMAN sp|P07476|INVO_HUMAN sp|P30086|PEBP1_HUMAN sp|P14923|PLAK_HUMAN sp|P00751|CFAB_HUMAN sp|P49913|CAMP_HUMAN sp|P40121|CAPG_HUMAN sp|P01772|HV311_HUMAN sp|Q86VR7-2|VS10L_HUMAN sp|P07108|ACBP_HUMAN sp|P04259|K2C6B_HUMAN sp|P02749|APOH_HUMAN sp|P15924|DESP_HUMAN sp|P04430|KV122_HUMAN sp|P00450|CERU_HUMAN sp|Q15323|K1H1_HUMAN sp|P28799|GRN_HUMAN sp|Q6FI13|H2A2A_HUMAN sp|P16401|H15_HUMAN sp|O00391|QSOX1_HUMAN sp|P02679|FIBG_HUMAN sp|P29373|RABP2_HUMAN sp|P31151|S10A7_HUMAN sp|P01781|HV320_HUMAN sp|P01033|TIMP1_HUMAN sp|P02790|HEMO_HUMAN sp|P35326|SPR2A_HUMAN sp|P06703|S10A6_HUMAN sp|Q9GZZ8|LACRT_HUMAN sp|P61769|B2MG_HUMAN sp|P08670|VIME_HUMAN sp|P06331|HV209_HUMAN sp|P30044|PRDX5_HUMAN sp|P04208|LV106_HUMAN sp|Q9NZT1|CALL5_HUMAN sp|P01717|LV403_HUMAN sp|Q9UKR3|KLK13_HUMAN sp|P02750|A2GL_HUMAN sp|P01743|HV102_HUMAN sp|P40926|MDHM_HUMAN sp|P41218|MNDA_HUMAN sp|P01011|AACT_HUMAN sp|P30041|PRDX6_HUMAN sp|P68871|HBB_HUMAN sp|P01773|HV312_HUMAN sp|Q14019|COTL1_HUMAN sp|P01861|IGHG4_HUMAN sp|P15153|RAC2_HUMAN sp|Q09666|AHNK_HUMAN sp|P22314|UBA1_HUMAN sp|P61158|ARP3_HUMAN sp|P0CG48|UBC_HUMAN sp|P12429|ANXA3_HUMAN sp|P62158|CALM_HUMAN sp|P00491|PNPH_HUMAN sp|P13489|RINI_HUMAN sp|P08571|CD14_HUMAN sp|P18669|PGAM1_HUMAN sp|P51149|RAB7A_HUMAN sp|P01703|LV105_HUMAN sp|P50395-2|GDIB_HUMAN sp|P0C0L5|CO4B_HUMAN sp|P61916|NPC2_HUMAN sp|P08727|K1C19_HUMAN sp|P01860|IGHG3_HUMAN sp|P31946|1433B_HUMAN sp|P62942|FKB1A_HUMAN sp|P30838|AL3A1_HUMAN sp|O14745|NHRF1_HUMAN sp|P48668|K2C6C_HUMAN sp|P0CF74|LAC6_HUMAN sp|Q9NSB4|KRT82_HUMAN sp|P22528|SPR1B_HUMAN sp|P01780|HV319_HUMAN sp|Q92876|KLK6_HUMAN sp|P11413-3|G6PD_HUMAN sp|Q14515|SPRL1_HUMAN sp|P40925-3|MDHC_HUMAN

Journal of Proteome Research

Alpha-1-antitrypsin OS=Homo sapiens GN=SERPINA1 PE=1 SV=3 2.6E-02 Calmodulin-like protein 3 OS=Homo sapiens GN=CALML3 PE=1 SV=2 2.2E-01 Desmoglein-1 OS=Homo sapiens GN=DSG1 PE=1 SV=2 9.9E-01 Histone H3.2 OS=Homo sapiens GN=HIST2H3A PE=1 SV=3 4.3E-02 Thymosin beta-4 OS=Homo sapiens GN=TMSB4X PE=1 SV=2 9.4E-01 Ig lambda chain V-III region LOI OS=Homo sapiens PE=1 SV=1 1.6E-01 Cathepsin G OS=Homo sapiens GN=CTSG PE=1 SV=2 2.7E-01 Heat shock protein beta-1 OS=Homo sapiens GN=HSPB1 PE=1 SV=2 3.7E-02 Thioredoxin OS=Homo sapiens GN=TXN PE=1 SV=3 4.6E-01 Rho GDP-dissociation inhibitor 2 OS=Homo sapiens GN=ARHGDIB PE=1 SV=3 6.9E-01 Kallikrein-1 OS=Homo sapiens GN=KLK1 PE=1 SV=2 1.1E-01 Peroxiredoxin-1 OS=Homo sapiens GN=PRDX1 PE=1 SV=1 1.7E-01 Heat shock cognate 71 kDa protein OS=Homo sapiens GN=HSPA8 PE=1 SV=1 7.2E-01 Protein-glutamine gamma-glutamyltransferase E OS=Homo sapiens GN=TGM3 PE=1 SV=4 6.5E-01 Adenylyl cyclase-associated protein 1 OS=Homo sapiens GN=CAP1 PE=1 SV=5 9.3E-01 WAP four-disulfide core domain protein 2 OS=Homo sapiens GN=WFDC2 PE=1 SV=2 2.4E-01 Transcobalamin-1 OS=Homo sapiens GN=TCN1 PE=1 SV=2 8.2E-01 Cystatin-A OS=Homo sapiens GN=CSTA PE=1 SV=1 2.7E-01 Cystatin-D OS=Homo sapiens GN=CST5 PE=1 SV=1 2.6E-02 Serpin B3 OS=Homo sapiens GN=SERPINB3 PE=1 SV=2 2.2E-01 Cornifin-A OS=Homo sapiens GN=SPRR1A PE=1 SV=2 8.4E-01 Catalase OS=Homo sapiens GN=CAT PE=1 SV=3 5.8E-02 Annexin A2 OS=Homo sapiens GN=ANXA2 PE=1 SV=2 3.2E-01 Ig lambda-2 chain C regions OS=Homo sapiens GN=IGLC2 PE=1 SV=1 1.0E-03 Peptidyl-prolyl cis-trans isomerase B OS=Homo sapiens GN=PPIB PE=1 SV=2 3.7E-01 Alpha-2-HS-glycoprotein OS=Homo sapiens GN=AHSG PE=1 SV=1 4.7E-01 Nucleobindin-2 OS=Homo sapiens GN=NUCB2 PE=1 SV=2 4.8E-04 Apolipoprotein A-II OS=Homo sapiens GN=APOA2 PE=1 SV=1 7.2E-01 Neutrophil defensin 3 OS=Homo sapiens GN=DEFA3 PE=1 SV=1 9.7E-01 Protein S100-P OS=Homo sapiens GN=S100P PE=1 SV=2 6.9E-01 Ig lambda chain V-III region SH OS=Homo sapiens PE=1 SV=1 4.8E-01 Ig kappa chain V-III region POM OS=Homo sapiens PE=1 SV=1 3.4E-01 Ig kappa chain V-I region EU OS=Homo sapiens PE=1 SV=1 5.4E-01 Keratin, type II cytoskeletal 2 epidermal OS=Homo sapiens GN=KRT2 PE=1 SV=2 4.6E-01 Ig kappa chain V-IV region B17 OS=Homo sapiens PE=2 SV=1 6.6E-01 Hemoglobin subunit alpha OS=Homo sapiens GN=HBA1 PE=1 SV=2 5.8E-02 Ig heavy chain V-III region VH26 OS=Homo sapiens PE=1 SV=1 8.4E-01 Cofilin-1 OS=Homo sapiens GN=CFL1 PE=1 SV=3 8.7E-01 Non-histone chromosomal protein HMG-17 OS=Homo sapiens GN=HMGN2 PE=1 SV=3 1.1E-03 Keratin, type I cytoskeletal 17 OS=Homo sapiens GN=KRT17 PE=1 SV=2 2.4E-01 Vinculin OS=Homo sapiens GN=VCL PE=1 SV=4 6.9E-01 Brain acid soluble protein 1 OS=Homo sapiens GN=BASP1 PE=1 SV=2 4.0E-01 Myosin-9 OS=Homo sapiens GN=MYH9 PE=1 SV=4 3.0E-01 Golgi membrane protein 1 OS=Homo sapiens GN=GOLM1 PE=1 SV=1 2.7E-03 Collagen alpha-2(I) chain OS=Homo sapiens GN=COL1A2 PE=1 SV=7 8.8E-01 Involucrin OS=Homo sapiens GN=IVL PE=1 SV=2 6.0E-01 Phosphatidylethanolamine-binding protein 1 OS=Homo sapiens GN=PEBP1 PE=1 SV=3 3.0E-01 Junction plakoglobin OS=Homo sapiens GN=JUP PE=1 SV=3 5.8E-01 Complement factor B OS=Homo sapiens GN=CFB PE=1 SV=2 9.6E-01 Cathelicidin antimicrobial peptide OS=Homo sapiens GN=CAMP PE=1 SV=1 6.1E-01 Macrophage-capping protein OS=Homo sapiens GN=CAPG PE=1 SV=2 5.9E-01 Ig heavy chain V-III region KOL OS=Homo sapiens PE=1 SV=1 4.8E-01 Isoform 2 of V-set and immunoglobulin domain-containing protein 10-like OS=Homo sapiens GN=VSIG10L 9.1E-01 Acyl-CoA-binding protein OS=Homo sapiens GN=DBI PE=1 SV=2 7.8E-01 Keratin, type II cytoskeletal 6B OS=Homo sapiens GN=KRT6B PE=1 SV=5 4.6E-02 Beta-2-glycoprotein 1 OS=Homo sapiens GN=APOH PE=1 SV=3 4.5E-01 Desmoplakin OS=Homo sapiens GN=DSP PE=1 SV=3 4.8E-01 Ig kappa chain V-I region BAN OS=Homo sapiens PE=1 SV=1 4.2E-01 Ceruloplasmin OS=Homo sapiens GN=CP PE=1 SV=1 8.0E-01 Keratin, type I cuticular Ha1 OS=Homo sapiens GN=KRT31 PE=2 SV=3 3.2E-01 Granulins OS=Homo sapiens GN=GRN PE=1 SV=2 3.2E-01 Histone H2A type 2-A OS=Homo sapiens GN=HIST2H2AA3 PE=1 SV=3 1.8E-02 Histone H1.5 OS=Homo sapiens GN=HIST1H1B PE=1 SV=3 3.1E-02 Sulfhydryl oxidase 1 OS=Homo sapiens GN=QSOX1 PE=1 SV=3 3.8E-01 Fibrinogen gamma chain OS=Homo sapiens GN=FGG PE=1 SV=3 6.3E-01 Cellular retinoic acid-binding protein 2 OS=Homo sapiens GN=CRABP2 PE=1 SV=2 5.0E-02 Protein S100-A7 OS=Homo sapiens GN=S100A7 PE=1 SV=4 2.9E-01 Ig heavy chain V-III region GAL OS=Homo sapiens PE=1 SV=1 5.2E-01 Metalloproteinase inhibitor 1 OS=Homo sapiens GN=TIMP1 PE=1 SV=1 9.8E-01 Hemopexin OS=Homo sapiens GN=HPX PE=1 SV=2 8.3E-01 Small proline-rich protein 2A OS=Homo sapiens GN=SPRR2A PE=2 SV=1 2.6E-01 Protein S100-A6 OS=Homo sapiens GN=S100A6 PE=1 SV=1 4.6E-02 Extracellular glycoprotein lacritin OS=Homo sapiens GN=LACRT PE=1 SV=1 1.3E-01 Beta-2-microglobulin OS=Homo sapiens GN=B2M PE=1 SV=1 5.8E-02 Vimentin OS=Homo sapiens GN=VIM PE=1 SV=4 6.4E-01 Ig heavy chain V-II region ARH-77 OS=Homo sapiens PE=4 SV=1 8.5E-01 Peroxiredoxin-5, mitochondrial OS=Homo sapiens GN=PRDX5 PE=1 SV=4 5.7E-01 Ig lambda chain V-I region WAH OS=Homo sapiens PE=1 SV=1 1.9E-01 Calmodulin-like protein 5 OS=Homo sapiens GN=CALML5 PE=1 SV=2 5.6E-01 Ig lambda chain V-IV region Hil OS=Homo sapiens PE=1 SV=1 7.0E-01 Kallikrein-13 OS=Homo sapiens GN=KLK13 PE=1 SV=1 4.8E-01 Leucine-rich alpha-2-glycoprotein OS=Homo sapiens GN=LRG1 PE=1 SV=2 1.0E+00 Ig heavy chain V-I region HG3 OS=Homo sapiens PE=4 SV=1 5.3E-02 Malate dehydrogenase, mitochondrial OS=Homo sapiens GN=MDH2 PE=1 SV=3 7.3E-01 Myeloid cell nuclear differentiation antigen OS=Homo sapiens GN=MNDA PE=1 SV=1 3.1E-01 Alpha-1-antichymotrypsin OS=Homo sapiens GN=SERPINA3 PE=1 SV=2 8.6E-02 Peroxiredoxin-6 OS=Homo sapiens GN=PRDX6 PE=1 SV=3 4.1E-01 Hemoglobin subunit beta OS=Homo sapiens GN=HBB PE=1 SV=2 2.9E-03 Ig heavy chain V-III region BUR OS=Homo sapiens PE=1 SV=1 9.1E-01 Coactosin-like protein OS=Homo sapiens GN=COTL1 PE=1 SV=3 4.4E-01 Ig gamma-4 chain C region OS=Homo sapiens GN=IGHG4 PE=1 SV=1 6.9E-01 Ras-related C3 botulinum toxin substrate 2 OS=Homo sapiens GN=RAC2 PE=1 SV=1 1.3E-01 Neuroblast differentiation-associated protein AHNAK OS=Homo sapiens GN=AHNAK PE=1 SV=2 1.7E-01 Ubiquitin-like modifier-activating enzyme 1 OS=Homo sapiens GN=UBA1 PE=1 SV=3 8.1E-01 Actin-related protein 3 OS=Homo sapiens GN=ACTR3 PE=1 SV=3 2.5E-01 Polyubiquitin-C OS=Homo sapiens GN=UBC PE=1 SV=3 2.3E-01 Annexin A3 OS=Homo sapiens GN=ANXA3 PE=1 SV=3 9.7E-01 Calmodulin OS=Homo sapiens GN=CALM1 PE=1 SV=2 4.0E-01 Purine nucleoside phosphorylase OS=Homo sapiens GN=PNP PE=1 SV=2 5.7E-01 Ribonuclease inhibitor OS=Homo sapiens GN=RNH1 PE=1 SV=2 5.4E-01 Monocyte differentiation antigen CD14 OS=Homo sapiens GN=CD14 PE=1 SV=2 2.9E-01 Phosphoglycerate mutase 1 OS=Homo sapiens GN=PGAM1 PE=1 SV=2 2.3E-01 Ras-related protein Rab-7a OS=Homo sapiens GN=RAB7A PE=1 SV=1 1.3E-01 Ig lambda chain V-I region NEWM OS=Homo sapiens PE=1 SV=1 5.5E-01 Isoform 2 of Rab GDP dissociation inhibitor beta OS=Homo sapiens GN=GDI2 7.7E-01 Complement C4-B OS=Homo sapiens GN=C4B PE=1 SV=2 9.4E-01 Epididymal secretory protein E1 OS=Homo sapiens GN=NPC2 PE=1 SV=1 7.2E-02 Keratin, type I cytoskeletal 19 OS=Homo sapiens GN=KRT19 PE=1 SV=4 3.3E-01 Ig gamma-3 chain C region OS=Homo sapiens GN=IGHG3 PE=1 SV=2 1.2E-01 14-3-3 protein beta/alpha OS=Homo sapiens GN=YWHAB PE=1 SV=3 6.4E-01 Peptidyl-prolyl cis-trans isomerase FKBP1A OS=Homo sapiens GN=FKBP1A PE=1 SV=2 9.7E-01 Aldehyde dehydrogenase, dimeric NADP-preferring OS=Homo sapiens GN=ALDH3A1 PE=1 SV=3 4.8E-01 Na(+)/H(+) exchange regulatory cofactor NHE-RF1 OS=Homo sapiens GN=SLC9A3R1 PE=1 SV=4 8.4E-01 Keratin, type II cytoskeletal 6C OS=Homo sapiens GN=KRT6C PE=1 SV=3 2.3E-01 Ig lambda-6 chain C region OS=Homo sapiens GN=IGLC6 PE=4 SV=1 5.4E-03 Keratin, type II cuticular Hb2 OS=Homo sapiens GN=KRT82 PE=1 SV=3 9.4E-01 Cornifin-B OS=Homo sapiens GN=SPRR1B PE=1 SV=2 5.1E-01 Ig heavy chain V-III region JON OS=Homo sapiens PE=1 SV=1 7.1E-01 Kallikrein-6 OS=Homo sapiens GN=KLK6 PE=1 SV=1 3.8E-02 Isoform 3 of Glucose-6-phosphate 1-dehydrogenase OS=Homo sapiens GN=G6PD 6.6E-01 SPARC-like protein 1 OS=Homo sapiens GN=SPARCL1 PE=1 SV=2 5.1E-01 Isoform 3 of Malate dehydrogenase, cytoplasmic OS=Homo sapiens GN=MDH1 4.7E-01

0.38 0.75 1.01 4.11 0.94 1.60 3.21 2.19 0.61 0.87 0.41 0.44 0.88 1.29 1.01 1.44 1.10 2.96 0.35 0.65 0.84 0.55 2.83 3.96 0.81 0.78 0.13 1.13 0.97 1.18 1.63 1.61 1.26 2.19 1.13 0.25 1.12 0.97 2.74 4.18 0.81 0.51 2.43 0.26 0.83 1.52 0.35 2.00 0.99 1.27 1.27 0.89 1.04 0.94 6.16 0.56 1.60 0.70 1.09 6.28 0.73 8.37 3.56 0.50 0.89 2.30 2.89 0.25 0.97 1.08 1.49 0.55 0.04 2.57 1.87 1.13 0.90 0.68 1.45 1.20 1.49 1.00 2.20 1.59 1.72 0.36 0.62 0.14 1.13 0.75 0.86 0.40 2.55 0.77 0.36 1.48 1.01 1.41 3.76 0.81 0.61 0.64 0.77 1.45 0.55 0.95 0.44 0.79 1.70 0.90 0.99 3.52 0.92 2.43 3.59 0.83 2.37 1.47 2.74 1.18 1.31 2.31

-0.42 -0.13 0.00 0.61 -0.03 0.20 0.51 0.34 -0.22 -0.06 -0.39 -0.35 -0.06 0.11 0.00 0.16 0.04 0.47 -0.46 -0.19 -0.08 -0.26 0.45 0.60 -0.09 -0.11 -0.90 0.05 -0.01 0.07 0.21 0.21 0.10 0.34 0.05 -0.61 0.05 -0.01 0.44 0.62 -0.09 -0.29 0.39 -0.58 -0.08 0.18 -0.46 0.30 0.00 0.10 0.10 -0.05 0.02 -0.03 0.79 -0.25 0.20 -0.15 0.04 0.80 -0.14 0.92 0.55 -0.30 -0.05 0.36 0.46 -0.61 -0.01 0.03 0.17 -0.26 -1.36 0.41 0.27 0.05 -0.05 -0.17 0.16 0.08 0.17 0.00 0.34 0.20 0.24 -0.44 -0.21 -0.86 0.05 -0.12 -0.07 -0.40 0.41 -0.11 -0.44 0.17 0.00 0.15 0.57 -0.09 -0.22 -0.19 -0.11 0.16 -0.26 -0.02 -0.36 -0.10 0.23 -0.05 0.00 0.55 -0.04 0.38 0.56 -0.08 0.37 0.17 0.44 0.07 0.12 0.36

11:11 9:9 8:8 11:11 7:7 11:11 4:4 7:7 9:9 11:11 13:13 9:9 9:9 15:15 11:11 15:15 11:11 5:5 11:11 11:11 9:9 11:11 2:2 15:15 13:13 9:9 5:5 5:5 13:13 5:5 8:8 6:6 13:13 6:6 9:9 9:9 7:7 9:9 9:9 3:3 7:7 7:7 2:2 9:9 3:3 3:3 5:5 2:2 5:5 11:11 5:5 9:9 4:4 3:3 8:8 7:7 4:4 3:3 9:9 2:2 7:7 3:3 7:7 4:4 13:13 5:5 5:5 3:3 5:5 13:13 6:6 15:15 2:2 9:9 8:8 3:3 2:2 13:13 2:2 11:11 5:5 2:2 15:15 7:7 2:2 8:8 7:7 11:11 2:2 10:10 13:13 8:8 5:5 5:5 4:4 5:5 2:2 5:5 3:3 6:6 8:8 4:4 2:2 2:2 2:2 2:2 7:7 2:2 14:14 5:5 2:2 2:2 6:6 10:10 11:11 2:2 5:5 2:2 4:4 5:5 3:3 4:4

ACS Paragon Plus Environment

5.6E-01 6.4E-01 7.0E-01 3.6E-01 9.4E-01 9.9E-01 9.3E-02 1.3E-01 6.4E-01 1.0E+00 1.9E-02 3.1E-01 5.0E-01 4.5E-01 4.9E-01 8.3E-01 6.2E-01 2.3E-01 4.9E-01 2.9E-01 7.3E-01 7.1E-01 1.4E-01 1.9E-01 9.2E-02 2.1E-01 2.9E-01 1.3E-01 7.7E-01 8.6E-01 4.8E-01 5.0E-01 5.9E-01 5.3E-01 7.2E-01 6.6E-01 7.4E-01 3.5E-01 1.4E-02 4.5E-01 9.6E-01 6.7E-01 1.7E-01 6.4E-01 7.4E-01 9.3E-01 9.5E-01 5.4E-01 1.6E-01 5.3E-01 9.7E-01 8.6E-01 7.9E-01 2.8E-01 2.4E-01 8.2E-01 3.9E-01 5.0E-01 7.5E-02 2.0E-01 4.4E-01 8.0E-03 3.1E-01 5.0E-01 2.7E-01 4.1E-01 4.0E-01 5.2E-01 4.9E-01 5.9E-01 2.4E-01 6.6E-01 3.1E-01 3.5E-01 6.0E-01 7.1E-01 2.1E-01 2.9E-01 5.0E-01 8.5E-01 7.2E-01 1.8E-01 1.3E-01 9.5E-01 3.4E-01 3.7E-01 7.1E-01 9.1E-01 2.6E-01 4.8E-01 7.3E-01 3.8E-01 3.6E-01 7.2E-01 7.2E-01 2.5E-01 4.7E-01 3.9E-01 5.4E-01 2.2E-01 4.9E-01 9.2E-01 1.2E-01 5.4E-01 2.0E-01 5.7E-01 2.5E-01 5.2E-01 1.0E-01 5.3E-01 7.5E-01 7.4E-01 8.0E-01 5.0E-01 9.3E-02 4.5E-01 4.8E-01 1.0E-01 7.2E-02 4.7E-01 7.8E-01 7.5E-01

0.76 0.87 1.25 1.86 0.94 1.01 3.03 2.59 0.74 1.00 0.25 0.56 1.32 1.50 1.21 1.09 0.81 1.57 0.68 0.65 0.73 0.89 2.26 1.68 1.76 1.42 0.45 2.23 1.20 1.21 1.65 1.25 1.20 2.36 0.92 1.20 0.86 1.37 2.33 2.96 0.97 0.72 4.81 1.22 0.68 0.93 0.93 2.52 3.88 1.37 1.01 1.05 1.22 1.75 3.18 0.84 1.91 0.75 1.85 22.70 1.83 10.09 1.80 0.55 1.36 1.73 2.83 0.24 1.54 1.37 1.62 1.25 0.18 1.66 2.07 1.60 1.32 0.74 1.79 0.92 1.28 0.59 1.95 0.92 6.19 0.56 0.83 1.06 0.42 1.44 0.84 0.57 1.81 0.69 0.70 1.89 3.94 2.34 4.38 0.63 0.66 1.05 0.73 1.43 0.09 0.59 0.55 2.33 1.85 1.29 1.15 1.21 1.11 1.66 2.42 8.47 2.46 0.35 2.28 0.77 1.14 0.77

-0.12 -0.06 0.10 0.27 -0.03 0.00 0.48 0.41 -0.13 0.00 -0.60 -0.25 0.12 0.18 0.08 0.04 -0.09 0.20 -0.17 -0.19 -0.14 -0.05 0.35 0.23 0.25 0.15 -0.34 0.35 0.08 0.08 0.22 0.10 0.08 0.37 -0.04 0.08 -0.07 0.14 0.37 0.47 -0.01 -0.14 0.68 0.09 -0.17 -0.03 -0.03 0.40 0.59 0.14 0.01 0.02 0.09 0.24 0.50 -0.07 0.28 -0.13 0.27 1.36 0.26 1.00 0.26 -0.26 0.13 0.24 0.45 -0.62 0.19 0.14 0.21 0.10 -0.75 0.22 0.32 0.20 0.12 -0.13 0.25 -0.03 0.11 -0.23 0.29 -0.04 0.79 -0.25 -0.08 0.03 -0.38 0.16 -0.07 -0.24 0.26 -0.16 -0.15 0.28 0.60 0.37 0.64 -0.20 -0.18 0.02 -0.14 0.16 -1.03 -0.23 -0.26 0.37 0.27 0.11 0.06 0.08 0.05 0.22 0.38 0.93 0.39 -0.46 0.36 -0.11 0.06 -0.12

11:11 9:9 8:8 11:11 7:7 11:11 4:4 7:7 9:9 11:11 13:13 9:9 9:9 15:15 11:11 15:15 11:11 5:5 11:11 11:11 9:9 11:11 2:2 15:15 13:13 9:9 5:5 5:5 13:13 5:5 8:8 6:6 13:13 6:6 9:9 9:9 7:7 9:9 9:9 3:3 7:7 7:7 2:2 9:9 3:3 3:3 5:5 2:2 5:5 11:11 5:5 9:9 4:4 3:3 8:8 7:7 4:4 3:3 9:9 2:2 7:7 3:3 7:7 4:4 13:13 5:5 5:5 3:3 5:5 13:13 6:6 15:15 2:2 9:9 8:8 3:3 2:2 13:13 2:2 11:11 5:5 2:2 15:15 7:7 2:2 8:8 7:7 11:11 2:2 10:10 13:13 8:8 5:5 5:5 4:4 5:5 2:2 5:5 3:3 6:6 8:8 4:4 2:2 2:2 2:2 2:2 7:7 2:2 14:14 5:5 2:2 2:2 6:6 10:10 11:11 2:2 5:5 2:2 4:4 5:5 3:3 4:4

1.3E-01 6.1E-01 7.1E-01 5.9E-02 1.0E+00 1.9E-01 9.6E-01 7.6E-01 7.9E-01 7.3E-01 2.1E-01 4.6E-01 2.9E-01 7.7E-01 5.1E-01 4.2E-01 4.3E-01 5.3E-01 1.7E-01 1.0E+00 8.6E-01 5.0E-02 8.2E-01 6.2E-02 1.8E-02 1.1E-01 9.2E-02 1.8E-01 6.5E-01 9.9E-01 9.9E-01 5.8E-01 8.9E-01 9.5E-01 4.8E-01 4.4E-02 5.5E-01 3.0E-01 5.5E-01 7.7E-01 7.6E-01 5.3E-01 5.4E-01 2.4E-04 7.8E-01 3.6E-01 1.4E-01 7.9E-01 1.4E-01 8.1E-01 6.2E-01 5.5E-01 8.3E-01 2.7E-01 4.0E-01 5.4E-01 8.4E-01 8.3E-01 1.5E-01 3.0E-01 2.6E-01 7.9E-01 7.0E-02 8.2E-01 1.6E-01 7.0E-01 9.8E-01 9.8E-01 6.4E-01 6.4E-01 7.6E-01 7.1E-02 4.1E-01 3.7E-01 9.5E-01 7.8E-01 8.7E-02 6.5E-01 7.0E-01 5.1E-01 7.7E-01 1.8E-01 7.9E-01 6.9E-01 4.8E-01 3.7E-01 7.1E-01 5.0E-03 3.5E-01 2.7E-01 9.5E-01 3.3E-01 6.9E-01 9.0E-01 3.1E-01 6.7E-01 4.8E-01 5.7E-01 9.5E-01 3.7E-01 8.7E-01 2.6E-01 7.0E-01 9.9E-01 3.4E-01 4.6E-01 5.7E-01 4.3E-01 7.7E-01 3.6E-01 7.6E-01 5.6E-01 6.1E-01 6.4E-01 3.1E-01 1.2E-02 9.8E-01 2.6E-01 7.3E-01 2.5E-01 7.2E-01 3.8E-01

0.49 0.86 0.80 2.22 1.00 1.59 1.06 0.84 0.82 0.87 1.65 0.79 0.66 0.86 0.83 1.33 1.36 1.89 0.52 1.00 1.15 0.62 1.25 2.35 0.46 0.55 0.28 0.50 0.81 0.98 0.99 1.29 1.04 0.93 1.23 0.21 1.30 0.71 1.18 1.41 0.83 0.71 0.51 0.22 1.22 1.63 0.37 0.79 0.25 0.93 1.25 0.85 0.85 0.54 1.93 0.66 0.84 0.94 0.59 0.28 0.40 0.83 1.98 0.90 0.65 1.33 1.02 1.04 0.63 0.79 0.92 0.44 0.25 1.55 0.91 0.71 0.68 0.92 0.81 1.30 1.17 1.68 1.13 1.72 0.28 0.64 0.75 0.13 2.69 0.52 1.02 0.70 1.41 1.12 0.52 0.78 0.26 0.60 0.86 1.27 0.92 0.61 1.05 1.01 5.94 1.61 0.81 0.34 0.92 0.70 0.86 2.90 0.83 1.47 1.49 0.10 0.96 4.23 1.21 1.53 1.15 3.02

-0.31 -0.07 -0.09 0.35 0.00 0.20 0.02 -0.07 -0.08 -0.06 0.22 -0.10 -0.18 -0.07 -0.08 0.12 0.13 0.28 -0.29 0.00 0.06 -0.21 0.10 0.37 -0.34 -0.26 -0.56 -0.30 -0.09 -0.01 -0.01 0.11 0.02 -0.03 0.09 -0.69 0.11 -0.15 0.07 0.15 -0.08 -0.15 -0.30 -0.66 0.09 0.21 -0.43 -0.10 -0.59 -0.03 0.10 -0.07 -0.07 -0.27 0.29 -0.18 -0.08 -0.03 -0.23 -0.56 -0.40 -0.08 0.30 -0.04 -0.18 0.12 0.01 0.02 -0.20 -0.10 -0.04 -0.35 -0.61 0.19 -0.04 -0.15 -0.17 -0.04 -0.09 0.11 0.07 0.23 0.05 0.24 -0.56 -0.19 -0.12 -0.89 0.43 -0.28 0.01 -0.15 0.15 0.05 -0.29 -0.11 -0.59 -0.22 -0.07 0.10 -0.04 -0.21 0.02 0.00 0.77 0.21 -0.09 -0.47 -0.04 -0.16 -0.07 0.46 -0.08 0.17 0.17 -1.01 -0.02 0.63 0.08 0.18 0.06 0.48

11:11 9:9 8:8 11:11 7:7 11:11 4:4 7:7 9:9 11:11 13:13 9:9 9:9 15:15 11:11 15:15 11:11 5:5 11:11 11:11 9:9 11:11 2:2 15:15 13:13 9:9 5:5 5:5 13:13 5:5 8:8 6:6 13:13 6:6 9:9 9:9 7:7 9:9 9:9 3:3 7:7 7:7 2:2 9:9 3:3 3:3 5:5 2:2 5:5 11:11 5:5 9:9 4:4 3:3 8:8 7:7 4:4 3:3 9:9 2:2 7:7 3:3 7:7 4:4 13:13 5:5 5:5 3:3 5:5 13:13 6:6 15:15 2:2 9:9 8:8 3:3 2:2 13:13 2:2 11:11 5:5 2:2 15:15 7:7 2:2 8:8 7:7 11:11 2:2 10:10 13:13 8:8 5:5 5:5 4:4 5:5 2:2 5:5 3:3 6:6 8:8 4:4 2:2 2:2 2:2 2:2 7:7 2:2 14:14 5:5 2:2 2:2 6:6 10:10 11:11 2:2 5:5 2:2 4:4 5:5 3:3 4:4

Journal of Proteome Research

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 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 60

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sp|P08246|ELNE_HUMAN sp|P07339|CATD_HUMAN sp|O75556|SG2A1_HUMAN sp|P47929|LEG7_HUMAN sp|P60660-2|MYL6_HUMAN sp|P33241|LSP1_HUMAN sp|Q8NEN0|ARMC2_HUMAN sp|P06316|LV107_HUMAN sp|O60664|PLIN3_HUMAN sp|P55058|PLTP_HUMAN sp|P07602|SAP_HUMAN sp|P01760|HV105_HUMAN sp|Q15149-9|PLEC_HUMAN sp|P01042|KNG1_HUMAN sp|Q92896-3|GSLG1_HUMAN sp|Q71U36|TBA1A_HUMAN sp|Q9H299|SH3L3_HUMAN sp|Q92817|EVPL_HUMAN sp|P58499|FAM3B_HUMAN sp|P78559|MAP1A_HUMAN sp|P59998|ARPC4_HUMAN sp|Q9UPS8-2|ANR26_HUMAN sp|Q16651|PRSS8_HUMAN sp|P08134|RHOC_HUMAN sp|P04155|TFF1_HUMAN sp|P31949|S10AB_HUMAN sp|P05107|ITB2_HUMAN sp|Q96HE7|ERO1A_HUMAN sp|Q6P4A8|PLBL1_HUMAN sp|P61981|1433G_HUMAN sp|P61604|CH10_HUMAN sp|Q02818|NUCB1_HUMAN sp|P14317|HCLS1_HUMAN sp|Q6NUI6-2|CHADL_HUMAN sp|P50552|VASP_HUMAN sp|P00441|SODC_HUMAN sp|P13987|CD59_HUMAN sp|Q9NQC3|RTN4_HUMAN sp|P81605|DCD_HUMAN sp|P26447|S10A4_HUMAN sp|P11684|UTER_HUMAN sp|P01768|HV307_HUMAN sp|Q9BWT7|CAR10_HUMAN sp|Q13421-2|MSLN_HUMAN sp|Q15847|ADIRF_HUMAN sp|Q9HCY8|S10AE_HUMAN sp|P24158|PRTN3_HUMAN sp|P01767|HV306_HUMAN sp|Q9UBR2|CATZ_HUMAN sp|P61160|ARP2_HUMAN sp|O15020-2|SPTN2_HUMAN sp|P01616|KV203_HUMAN sp|Q99497|PARK7_HUMAN sp|P01621|KV303_HUMAN sp|P27348|1433T_HUMAN sp|O76013|KRT36_HUMAN sp|Q15485|FCN2_HUMAN RRRRRsp|Q8TD17|ZN398_HUMAN sp|P23083|HV103_HUMAN sp|Q9BRK5|CAB45_HUMAN sp|P22392-2|NDKB_HUMAN sp|Q9ULD4|BRPF3_HUMAN sp|P36952|SPB5_HUMAN sp|P02763|A1AG1_HUMAN sp|P61026|RAB10_HUMAN sp|P78417|GSTO1_HUMAN sp|O95968|SG1D1_HUMAN sp|P54727|RD23B_HUMAN sp|Q15907|RB11B_HUMAN sp|P22626|ROA2_HUMAN sp|P16870|CBPE_HUMAN sp|P63218|GBG5_HUMAN sp|Q13835|PKP1_HUMAN sp|O95467|GNAS3_HUMAN sp|O60500|NPHN_HUMAN sp|P01621|KV303_HUMAN sp|P27348|1433T_HUMAN sp|O76013|KRT36_HUMAN sp|Q15485|FCN2_HUMAN sp|Q86UQ4|ABCAD_HUMAN RRRRRsp|Q8TD17|ZN398_HUMAN sp|Q9Y446|PKP3_HUMAN sp|P23083|HV103_HUMAN sp|Q5SVZ6|ZMYM1_HUMAN sp|Q8IZD4|DCP1B_HUMAN sp|Q9BRK5|CAB45_HUMAN sp|P22392-2|NDKB_HUMAN sp|Q5VTE0|EF1A3_HUMAN sp|Q9ULD4|BRPF3_HUMAN sp|P36952|SPB5_HUMAN sp|P02763|A1AG1_HUMAN sp|P61026|RAB10_HUMAN sp|Q9UHB6|LIMA1_HUMAN sp|P78417|GSTO1_HUMAN sp|Q9H7C4|SYNCI_HUMAN sp|O95968|SG1D1_HUMAN sp|P54727|RD23B_HUMAN sp|Q2KJY2|KI26B_HUMAN sp|Q15907|RB11B_HUMAN sp|P61978|HNRPK_HUMAN sp|Q6ZTR5|CX022_HUMAN sp|P22626|ROA2_HUMAN sp|Q9UP95-7|S12A4_HUMAN sp|P16870|CBPE_HUMAN sp|Q9NPI8|FANCF_HUMAN sp|P63218|GBG5_HUMAN sp|Q13835|PKP1_HUMAN sp|P16989|YBOX3_HUMAN sp|O95467|GNAS3_HUMAN

Neutrophil elastase OS=Homo sapiens GN=ELANE PE=1 SV=1 5.7E-01 Cathepsin D OS=Homo sapiens GN=CTSD PE=1 SV=1 9.6E-01 Mammaglobin-B OS=Homo sapiens GN=SCGB2A1 PE=1 SV=1 1.2E-01 Galectin-7 OS=Homo sapiens GN=LGALS7 PE=1 SV=2 8.1E-01 Isoform Smooth muscle of Myosin light polypeptide 6 OS=Homo sapiens GN=MYL6 8.2E-01 Lymphocyte-specific protein 1 OS=Homo sapiens GN=LSP1 PE=1 SV=1 4.1E-01 Armadillo repeat-containing protein 2 OS=Homo sapiens GN=ARMC2 PE=2 SV=4 8.8E-01 Ig lambda chain V-I region BL2 OS=Homo sapiens PE=2 SV=1 5.8E-01 Perilipin-3 OS=Homo sapiens GN=PLIN3 PE=1 SV=3 3.3E-01 Phospholipid transfer protein OS=Homo sapiens GN=PLTP PE=1 SV=1 2.8E-02 Proactivator polypeptide OS=Homo sapiens GN=PSAP PE=1 SV=2 3.2E-01 Ig heavy chain V-I region WOL OS=Homo sapiens PE=1 SV=1 6.7E-01 Isoform 9 of Plectin OS=Homo sapiens GN=PLEC 4.9E-01 Kininogen-1 OS=Homo sapiens GN=KNG1 PE=1 SV=2 1.9E-01 Isoform 3 of Golgi apparatus protein 1 OS=Homo sapiens GN=GLG1 6.8E-01 Tubulin alpha-1A chain OS=Homo sapiens GN=TUBA1A PE=1 SV=1 4.5E-01 SH3 domain-binding glutamic acid-rich-like protein 3 OS=Homo sapiens GN=SH3BGRL3 PE=1 SV=1 7.5E-01 Envoplakin OS=Homo sapiens GN=EVPL PE=1 SV=3 1.1E-01 Protein FAM3B OS=Homo sapiens GN=FAM3B PE=1 SV=2 4.4E-01 Microtubule-associated protein 1A OS=Homo sapiens GN=MAP1A PE=1 SV=6 2.8E-01 Actin-related protein 2/3 complex subunit 4 OS=Homo sapiens GN=ARPC4 PE=1 SV=3 2.9E-02 Isoform 2 of Ankyrin repeat domain-containing protein 26 OS=Homo sapiens GN=ANKRD26 3.5E-01 Prostasin OS=Homo sapiens GN=PRSS8 PE=1 SV=1 6.2E-01 Rho-related GTP-binding protein RhoC OS=Homo sapiens GN=RHOC PE=1 SV=1 8.9E-01 Trefoil factor 1 OS=Homo sapiens GN=TFF1 PE=1 SV=1 6.9E-01 Protein S100-A11 OS=Homo sapiens GN=S100A11 PE=1 SV=2 5.5E-01 Integrin beta-2 OS=Homo sapiens GN=ITGB2 PE=1 SV=2 7.8E-01 ERO1-like protein alpha OS=Homo sapiens GN=ERO1L PE=1 SV=2 8.3E-01 Phospholipase B-like 1 OS=Homo sapiens GN=PLBD1 PE=1 SV=2 4.9E-01 14-3-3 protein gamma OS=Homo sapiens GN=YWHAG PE=1 SV=2 7.8E-01 10 kDa heat shock protein, mitochondrial OS=Homo sapiens GN=HSPE1 PE=1 SV=2 3.3E-01 Nucleobindin-1 OS=Homo sapiens GN=NUCB1 PE=1 SV=4 1.5E-01 Hematopoietic lineage cell-specific protein OS=Homo sapiens GN=HCLS1 PE=1 SV=3 5.3E-01 Isoform 2 of Chondroadherin-like protein OS=Homo sapiens GN=CHADL 1.5E-01 Vasodilator-stimulated phosphoprotein OS=Homo sapiens GN=VASP PE=1 SV=3 1.0E-01 Superoxide dismutase [Cu-Zn] OS=Homo sapiens GN=SOD1 PE=1 SV=2 2.6E-01 CD59 glycoprotein OS=Homo sapiens GN=CD59 PE=1 SV=1 7.4E-01 Reticulon-4 OS=Homo sapiens GN=RTN4 PE=1 SV=2 9.9E-01 Dermcidin OS=Homo sapiens GN=DCD PE=1 SV=2 3.7E-02 Protein S100-A4 OS=Homo sapiens GN=S100A4 PE=1 SV=1 4.7E-01 Uteroglobin OS=Homo sapiens GN=SCGB1A1 PE=1 SV=1 3.8E-02 Ig heavy chain V-III region CAM OS=Homo sapiens PE=1 SV=1 7.3E-01 Caspase recruitment domain-containing protein 10 OS=Homo sapiens GN=CARD10 PE=2 SV=2 1.7E-01 Isoform 3 of Mesothelin OS=Homo sapiens GN=MSLN 3.1E-01 Adipogenesis regulatory factor OS=Homo sapiens GN=ADIRF PE=1 SV=1 2.5E-01 Protein S100-A14 OS=Homo sapiens GN=S100A14 PE=1 SV=1 3.1E-01 Myeloblastin OS=Homo sapiens GN=PRTN3 PE=1 SV=3 1.6E-01 Ig heavy chain V-III region BUT OS=Homo sapiens PE=1 SV=1 8.6E-01 Cathepsin Z OS=Homo sapiens GN=CTSZ PE=1 SV=1 4.7E-01 Actin-related protein 2 OS=Homo sapiens GN=ACTR2 PE=1 SV=1 1.6E-01 Isoform 2 of Spectrin beta chain, non-erythrocytic 2 OS=Homo sapiens GN=SPTBN2 2.0E-01 Ig kappa chain V-II region MIL OS=Homo sapiens PE=1 SV=1 3.8E-01 Protein DJ-1 OS=Homo sapiens GN=PARK7 PE=1 SV=2 9.8E-01 Ig kappa chain V-III region NG9 (Fragment) OS=Homo sapiens PE=1 SV=1 4.0E-02 14-3-3 protein theta OS=Homo sapiens GN=YWHAQ PE=1 SV=1 3.5E-01 Keratin, type I cuticular Ha6 OS=Homo sapiens GN=KRT36 PE=1 SV=1 1.7E-01 Ficolin-2 OS=Homo sapiens GN=FCN2 PE=1 SV=2 3.4E-01 REVERSED Zinc finger protein 398 OS=Homo sapiens GN=ZNF398 PE=2 SV=1 9.8E-02 Ig heavy chain V-I region V35 OS=Homo sapiens PE=1 SV=1 1.3E-01 45 kDa calcium-binding protein OS=Homo sapiens GN=SDF4 PE=1 SV=1 8.1E-01 Isoform 3 of Nucleoside diphosphate kinase B OS=Homo sapiens GN=NME2 8.2E-03 Bromodomain and PHD finger-containing protein 3 OS=Homo sapiens GN=BRPF3 PE=1 SV=2 3.9E-01 Serpin B5 OS=Homo sapiens GN=SERPINB5 PE=1 SV=2 4.7E-01 Alpha-1-acid glycoprotein 1 OS=Homo sapiens GN=ORM1 PE=1 SV=1 3.6E-01 Ras-related protein Rab-10 OS=Homo sapiens GN=RAB10 PE=1 SV=1 8.8E-01 Glutathione S-transferase omega-1 OS=Homo sapiens GN=GSTO1 PE=1 SV=2 6.1E-01 Secretoglobin family 1D member 1 OS=Homo sapiens GN=SCGB1D1 PE=1 SV=1 2.6E-01 UV excision repair protein RAD23 homolog B OS=Homo sapiens GN=RAD23B PE=1 SV=1 6.4E-01 Ras-related protein Rab-11B OS=Homo sapiens GN=RAB11B PE=1 SV=4 8.9E-01 Heterogeneous nuclear ribonucleoproteins A2/B1 OS=Homo sapiens GN=HNRNPA2B1 PE=1 SV=2 9.2E-01 Carboxypeptidase E OS=Homo sapiens GN=CPE PE=1 SV=1 1.1E-01 Guanine nucleotide-binding protein G(I)/G(S)/G(O) subunit gamma-5 OS=Homo sapiens GN=GNG5 PE=1 SV=3 4.3E-01 Plakophilin-1 OS=Homo sapiens GN=PKP1 PE=1 SV=2 4.4E-01 Neuroendocrine secretory protein 55 OS=Homo sapiens GN=GNAS PE=1 SV=1 8.0E-01 Nephrin OS=Homo sapiens GN=NPHS1 PE=1 SV=1 Ig kappa chain V-III region NG9 (Fragment) OS=Homo sapiens PE=1 SV=1 14-3-3 protein theta OS=Homo sapiens GN=YWHAQ PE=1 SV=1 Keratin, type I cuticular Ha6 OS=Homo sapiens GN=KRT36 PE=1 SV=1 Ficolin-2 OS=Homo sapiens GN=FCN2 PE=1 SV=2 ATP-binding cassette sub-family A member 13 OS=Homo sapiens GN=ABCA13 PE=2 SV=3 REVERSED Zinc finger protein 398 OS=Homo sapiens GN=ZNF398 PE=2 SV=1 Plakophilin-3 OS=Homo sapiens GN=PKP3 PE=1 SV=1 Ig heavy chain V-I region V35 OS=Homo sapiens PE=1 SV=1 Zinc finger MYM-type protein 1 OS=Homo sapiens GN=ZMYM1 PE=2 SV=1 mRNA-decapping enzyme 1B OS=Homo sapiens GN=DCP1B PE=1 SV=2 45 kDa calcium-binding protein OS=Homo sapiens GN=SDF4 PE=1 SV=1 Isoform 3 of Nucleoside diphosphate kinase B OS=Homo sapiens GN=NME2 Putative elongation factor 1-alpha-like 3 OS=Homo sapiens GN=EEF1A1P5 PE=5 SV=1 Bromodomain and PHD finger-containing protein 3 OS=Homo sapiens GN=BRPF3 PE=1 SV=2 Serpin B5 OS=Homo sapiens GN=SERPINB5 PE=1 SV=2 Alpha-1-acid glycoprotein 1 OS=Homo sapiens GN=ORM1 PE=1 SV=1 Ras-related protein Rab-10 OS=Homo sapiens GN=RAB10 PE=1 SV=1 LIM domain and actin-binding protein 1 OS=Homo sapiens GN=LIMA1 PE=1 SV=1 Glutathione S-transferase omega-1 OS=Homo sapiens GN=GSTO1 PE=1 SV=2 Syncoilin OS=Homo sapiens GN=SYNC PE=1 SV=3 Secretoglobin family 1D member 1 OS=Homo sapiens GN=SCGB1D1 PE=1 SV=1 UV excision repair protein RAD23 homolog B OS=Homo sapiens GN=RAD23B PE=1 SV=1 Kinesin-like protein KIF26B OS=Homo sapiens GN=KIF26B PE=2 SV=1 Ras-related protein Rab-11B OS=Homo sapiens GN=RAB11B PE=1 SV=4 Heterogeneous nuclear ribonucleoprotein K OS=Homo sapiens GN=HNRNPK PE=1 SV=1 Uncharacterized protein CXorf22 OS=Homo sapiens GN=CXorf22 PE=2 SV=3 Heterogeneous nuclear ribonucleoproteins A2/B1 OS=Homo sapiens GN=HNRNPA2B1 PE=1 SV=2 Isoform 7 of Solute carrier family 12 member 4 OS=Homo sapiens GN=SLC12A4 Carboxypeptidase E OS=Homo sapiens GN=CPE PE=1 SV=1 Fanconi anemia group F protein OS=Homo sapiens GN=FANCF PE=1 SV=1 Guanine nucleotide-binding protein G(I)/G(S)/G(O) subunit gamma-5 OS=Homo sapiens GN=GNG5 PE=1 SV=3 Plakophilin-1 OS=Homo sapiens GN=PKP1 PE=1 SV=2 Y-box-binding protein 3 OS=Homo sapiens GN=YBX3 PE=1 SV=4 Neuroendocrine secretory protein 55 OS=Homo sapiens GN=GNAS PE=1 SV=1

0.66 0.94 0.03 1.15 1.12 0.58 1.11 1.39 0.78 0.51 0.66 1.86 1.37 0.34 0.63 2.56 1.25 10.14 0.73 1.61 1.72 0.51 1.21 0.90 0.88 0.87 1.18 1.48 1.35 1.24 0.67 0.58 0.71 1.50 0.42 1.14 1.61 1.01 0.31 1.27 0.30 1.10 1.52 0.37 0.60 4.66 4.34 0.88 0.56 2.11 2.38 1.51 1.02 2.21 0.45 3.30 1.93 0.14 1.54 0.79 0.95 1.55 0.81 1.55 1.13 0.77 0.34 1.83 1.19 1.07 0.61 0.72 1.55 1.38

-0.18 -0.03 -1.59 0.06 0.05 -0.24 0.05 0.14 -0.11 -0.30 -0.18 0.27 0.14 -0.47 -0.20 0.41 0.10 1.01 -0.14 0.21 0.24 -0.29 0.08 -0.04 -0.05 -0.06 0.07 0.17 0.13 0.09 -0.17 -0.23 -0.15 0.18 -0.38 0.06 0.21 0.00 -0.51 0.10 -0.52 0.04 0.18 -0.44 -0.23 0.67 0.64 -0.06 -0.25 0.32 0.38 0.18 0.01 0.34 -0.35 0.52 0.29 -0.87 0.19 -0.10 -0.02 0.19 -0.09 0.19 0.05 -0.11 -0.47 0.26 0.08 0.03 -0.22 -0.14 0.19 0.14

4:4 7:7 2:2 2:2 4:4 9:9 8:8 11:11 3:3 9:9 11:11 6:6 7:7 3:3 2:2 2:2 6:6 2:2 6:6 2:2 3:3 7:7 2:2 5:5 2:2 15:15 4:4 3:3 2:2 4:4 2:2 3:3 2:2 10:10 2:2 3:3 2:2 3:3 2:2 5:5 6:6 2:2 2:2 3:3 3:3 2:2 5:5 4:4 2:2 2:2 2:2 2:2 3:3 11:11 4:4 2:2 2:2 2:2 9:9 4:4 2:2 2:2 5:5 10:10 2:2 10:10 2:2 2:2 7:7 2:2 2:2 2:2 2:2 2:2

ACS Paragon Plus Environment

Page 16 of 26

4.8E-01 9.6E-01 4.5E-01 9.9E-01 6.0E-01 6.5E-01 5.9E-01 9.4E-01 5.7E-01 2.2E-01 9.5E-01 8.2E-01 8.5E-01 8.3E-01 4.8E-01 3.4E-03 6.0E-01 2.6E-02 4.4E-01 3.2E-01 5.0E-03 2.6E-01 5.9E-01 8.4E-01 2.4E-01 7.3E-01 3.2E-01 3.8E-01 6.9E-01 5.9E-01 4.8E-01 8.5E-01 2.9E-01 3.9E-01 3.8E-01 6.6E-01 4.0E-01 5.6E-01 5.4E-01 1.1E-01 3.2E-01 7.6E-02 7.7E-02 8.9E-01 1.7E-01 9.9E-01 9.4E-01 8.7E-01 2.3E-01 6.7E-01 2.0E-01 3.8E-01 8.6E-01 1.2E-01 8.1E-01 7.1E-02 2.4E-01 1.5E-01 4.2E-01 5.7E-01 8.3E-01 2.2E-01 3.4E-01 6.5E-01 9.5E-01 7.1E-01 5.3E-01 4.5E-01 8.4E-01 3.2E-01 2.2E-01 3.8E-01 8.8E-01 9.2E-01

1.99 0.95 0.41 1.00 0.87 0.75 1.48 0.95 1.12 0.69 0.97 1.38 1.08 0.85 0.43 3.31 0.68 7.91 1.45 1.82 2.64 0.43 0.81 1.15 1.80 1.10 1.68 0.54 0.90 1.49 5.11 0.91 0.49 1.32 0.56 0.88 0.69 1.25 4.37 2.47 0.53 0.58 1.71 1.21 0.60 1.01 1.05 1.12 0.52 0.74 3.27 0.63 1.16 1.68 0.77 4.31 3.48 0.15 1.44 2.15 0.96 2.18 1.86 1.30 0.94 0.83 1.22 0.58 1.28 0.73 0.65 8.20 0.87 0.88

0.30 -0.02 -0.38 0.00 -0.06 -0.12 0.17 -0.02 0.05 -0.16 -0.01 0.14 0.03 -0.07 -0.36 0.52 -0.16 0.90 0.16 0.26 0.42 -0.37 -0.09 0.06 0.26 0.04 0.23 -0.27 -0.05 0.17 0.71 -0.04 -0.31 0.12 -0.25 -0.05 -0.16 0.10 0.64 0.39 -0.27 -0.24 0.23 0.08 -0.22 0.00 0.02 0.05 -0.29 -0.13 0.51 -0.20 0.06 0.23 -0.11 0.63 0.54 -0.82 0.16 0.33 -0.02 0.34 0.27 0.11 -0.03 -0.08 0.09 -0.23 0.11 -0.13 -0.19 0.91 -0.06 -0.05

4:4 7:7 2:2 2:2 4:4 9:9 8:8 11:11 3:3 9:9 11:11 6:6 7:7 3:3 2:2 2:2 6:6 2:2 6:6 2:2 3:3 7:7 2:2 5:5 2:2 15:15 4:4 3:3 2:2 4:4 2:2 3:3 2:2 10:10 2:2 3:3 2:2 3:3 2:2 5:5 6:6 2:2 2:2 3:3 3:3 2:2 5:5 4:4 2:2 2:2 2:2 2:2 3:3 11:11 4:4 2:2 2:2 2:2 9:9 4:4 2:2 2:2 5:5 10:10 2:2 10:10 2:2 2:2 7:7 2:2 2:2 2:2 2:2 2:2

1.3E-01 9.9E-01 2.4E-01 7.8E-01 6.2E-01 6.5E-01 6.7E-01 5.1E-01 1.5E-01 2.9E-01 4.0E-01 8.5E-01 5.6E-01 1.2E-01 1.5E-01 8.2E-01 3.9E-01 8.0E-01 2.4E-01 8.4E-01 1.3E-01 6.7E-01 2.1E-01 7.3E-01 1.1E-01 3.6E-01 3.1E-01 5.6E-01 3.2E-01 8.6E-01 3.9E-01 3.2E-01 4.6E-01 5.9E-01 5.5E-01 4.1E-01 5.6E-01 6.2E-01 3.2E-01 2.3E-01 2.5E-01 1.5E-01 4.8E-01 2.8E-01 9.5E-01 3.3E-01 1.8E-01 7.8E-01 9.1E-01 2.3E-01 7.0E-01 5.4E-02 8.8E-01 3.4E-01 5.4E-01 5.5E-01 4.7E-01 9.2E-01 8.8E-01 4.7E-01 9.3E-01 2.1E-01 2.2E-01 7.6E-01 8.3E-01 8.5E-01 1.9E-01 3.5E-01 9.6E-01 6.1E-01 7.8E-01 3.3E-01 5.4E-01 4.5E-01

0.33 0.99 0.06 1.15 1.29 0.77 0.75 1.46 0.70 0.74 0.68 1.34 1.27 0.40 1.45 0.77 1.82 1.28 0.51 0.88 0.65 1.20 1.50 0.78 0.49 0.79 0.70 2.75 1.51 0.84 0.13 0.64 1.46 1.14 0.74 1.29 2.34 0.80 0.07 0.52 0.56 1.89 0.89 0.30 0.98 4.61 4.15 0.78 1.09 2.83 0.73 2.39 0.88 1.32 0.58 0.77 0.55 0.90 1.07 0.37 0.99 0.71 0.44 1.20 1.20 0.93 0.28 3.13 0.93 1.46 0.94 0.09 1.77 1.56

-0.48 0.00 -1.21 0.06 0.11 -0.11 -0.12 0.16 -0.16 -0.13 -0.17 0.13 0.10 -0.40 0.16 -0.11 0.26 0.11 -0.30 -0.05 -0.19 0.08 0.18 -0.11 -0.31 -0.10 -0.15 0.44 0.18 -0.08 -0.88 -0.19 0.16 0.06 -0.13 0.11 0.37 -0.09 -1.15 -0.29 -0.25 0.28 -0.05 -0.52 -0.01 0.66 0.62 -0.11 0.04 0.45 -0.14 0.38 -0.06 0.12 -0.24 -0.12 -0.26 -0.05 0.03 -0.44 -0.01 -0.15 -0.36 0.08 0.08 -0.03 -0.56 0.50 -0.03 0.16 -0.03 -1.05 0.25 0.19

4:4 7:7 2:2 2:2 4:4 9:9 8:8 11:11 3:3 9:9 11:11 6:6 7:7 3:3 2:2 2:2 6:6 2:2 6:6 2:2 3:3 7:7 2:2 5:5 2:2 15:15 4:4 3:3 2:2 4:4 2:2 3:3 2:2 10:10 2:2 3:3 2:2 3:3 2:2 5:5 6:6 2:2 2:2 3:3 3:3 2:2 5:5 4:4 2:2 2:2 2:2 2:2 3:3 11:11 4:4 2:2 2:2 2:2 9:9 4:4 2:2 2:2 5:5 10:10 2:2 10:10 2:2 2:2 7:7 2:2 2:2 2:2 2:2 2:2

Page 17 of 26

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48

Journal of Proteome Research

Table S-2. Comparison of differentially expressed proteins among donor groups (p < 0.05) PS, pSS vs. HC Master N

Accession Number

Gene Name

17 24 97 140 191 115 18 34 20 98 74 42 64 61 145 218 68 15 5 30 26 6 67 1 2 43 77 81 76 48 10 21 44 46 62 79 137 151 55 29 120 27

P01857 P0CG05 P61769 P01859 P01700 P04208 P01834 P01009 P01871 P04433 B9A064 Q08380 P01011 P80188 P01780 P00736 P06309 P02787 P01833 P01591 P10909-2 P02788 Q14508 P04745 P02810 P02808 P52209 P23284 P01609 P80303 P22079 P13645 Q8TDL5 P35908 P07237 P08123 P02750 Q8N4F0 P04080 P15515 P35321 Q96DR5

IGHG1_HUMAN LAC2_HUMAN B2MG_HUMAN IGHG2_HUMAN LV102_HUMAN LV106_HUMAN IGKC_HUMAN A1AT_HUMAN IGHM_HUMAN KV309_HUMAN IGLL5_HUMAN LG3BP_HUMAN AACT_HUMAN NGAL_HUMAN HV319_HUMAN C1R_HUMAN KV205_HUMAN TRFE_HUMAN PIGR_HUMAN IGJ_HUMAN CLUS_HUMAN TRFL_HUMAN WFDC2_HUMAN AMY1_HUMAN PRPC_HUMAN STAT_HUMAN 6PGD_HUMAN PPIB_HUMAN KV117_HUMAN NUCB2_HUMAN PERL_HUMAN K1C10_HUMAN BPIB1_HUMAN K22E_HUMAN PDIA1_HUMAN CO1A2_HUMAN A2GL_HUMAN BPIB2_HUMAN CYTB_HUMAN HIS1_HUMAN SPR1A_HUMAN BPIA2_HUMAN

Protein Name Ig gamma-1 chain C region OS=Homo sapiens GN=IGHG1 PE=1 SV=1 Ig lambda-2 chain C regions OS=Homo sapiens GN=IGLC2 PE=1 SV=1 Beta-2-microglobulin OS=Homo sapiens GN=B2M PE=1 SV=1 Ig gamma-2 chain C region OS=Homo sapiens GN=IGHG2 PE=1 SV=2 Ig lambda chain V-I region HA OS=Homo sapiens PE=1 SV=1 Ig lambda chain V-I region WAH OS=Homo sapiens PE=1 SV=1 Ig kappa chain C region OS=Homo sapiens GN=IGKC PE=1 SV=1 Alpha-1-antitrypsin OS=Homo sapiens GN=SERPINA1 PE=1 SV=3 Ig mu chain C region OS=Homo sapiens GN=IGHM PE=1 SV=3 Ig kappa chain V-III region VG (Fragment) OS=Homo sapiens PE=1 SV=1 Immunoglobulin lambda-like polypeptide 5 OS=Homo sapiens GN=IGLL5 PE=2 SV=2 Galectin-3-binding protein OS=Homo sapiens GN=LGALS3BP PE=1 SV=1 Alpha-1-antichymotrypsin OS=Homo sapiens GN=SERPINA3 PE=1 SV=2 Neutrophil gelatinase-associated lipocalin OS=Homo sapiens GN=LCN2 PE=1 SV=2 Ig heavy chain V-III region JON OS=Homo sapiens PE=1 SV=1 Complement C1r subcomponent OS=Homo sapiens GN=C1R PE=1 SV=2 Ig kappa chain V-II region GM607 (Fragment) OS=Homo sapiens PE=4 SV=1 Serotransferrin OS=Homo sapiens GN=TF PE=1 SV=3 Polymeric immunoglobulin receptor OS=Homo sapiens GN=PIGR PE=1 SV=4 Immunoglobulin J chain OS=Homo sapiens GN=IGJ PE=1 SV=4 Isoform 2 of Clusterin OS=Homo sapiens GN=CLU Lactotransferrin OS=Homo sapiens GN=LTF PE=1 SV=6 WAP four-disulfide core domain protein 2 OS=Homo sapiens GN=WFDC2 PE=1 SV=2 Alpha-amylase 1 OS=Homo sapiens GN=AMY1A PE=1 SV=2 Salivary acidic proline-rich phosphoprotein 1/2 OS=Homo sapiens GN=PRH1 PE=1 SV=2 Statherin OS=Homo sapiens GN=STATH PE=1 SV=2 6-phosphogluconate dehydrogenase, decarboxylating OS=Homo sapiens GN=PGD PE=1 SV=3 Peptidyl-prolyl cis-trans isomerase B OS=Homo sapiens GN=PPIB PE=1 SV=2 Ig kappa chain V-I region Scw OS=Homo sapiens PE=1 SV=1 Nucleobindin-2 OS=Homo sapiens GN=NUCB2 PE=1 SV=2 Lactoperoxidase OS=Homo sapiens GN=LPO PE=1 SV=2 Keratin, type I cytoskeletal 10 OS=Homo sapiens GN=KRT10 PE=1 SV=6 BPI fold-containing family B member 1 OS=Homo sapiens GN=BPIFB1 PE=2 SV=1 Keratin, type II cytoskeletal 2 epidermal OS=Homo sapiens GN=KRT2 PE=1 SV=2 Protein disulfide-isomerase OS=Homo sapiens GN=P4HB PE=1 SV=3 Collagen alpha-2(I) chain OS=Homo sapiens GN=COL1A2 PE=1 SV=7 Leucine-rich alpha-2-glycoprotein OS=Homo sapiens GN=LRG1 PE=1 SV=2 BPI fold-containing family B member 2 OS=Homo sapiens GN=BPIFB2 PE=1 SV=2 Cystatin-B OS=Homo sapiens GN=CSTB PE=1 SV=2 Histatin-1 OS=Homo sapiens GN=HTN1 PE=1 SV=2 Cornifin-A OS=Homo sapiens GN=SPRR1A PE=1 SV=2 BPI fold-containing family A member 2 OS=Homo sapiens GN=BPIFA2 PE=1 SV=2

ACS Paragon Plus Environment

pSS / HC pSS / HC pSS / HC pSS / HC ttest fold lin fold log n1-n2 7.7E-04 1.3E-09 1.5E-02 6.3E-03 3.3E-02 7.4E-03 1.8E-03 3.5E-02 3.2E-03 1.1E-02 8.7E-04 1.0E-04 4.4E-02 1.1E-02 2.0E-02 4.3E-02 7.3E-03 9.9E-03 1.6E-02 5.5E-03 1.1E-03 2.2E-02 3.2E-02 2.9E-03 4.7E-02 2.8E-02 4.1E-02 2.4E-02 4.3E-02 3.9E-02 7.7E-03 3.1E-02 1.6E-02 3.2E-02 1.8E-02 2.6E-02 1.9E-02 2.8E-02 6.7E-03 3.1E-04 4.5E-02 6.9E-04

6.20 5.33 4.05 3.83 3.65 3.53 3.52 3.36 3.15 3.05 2.98 2.81 2.79 2.72 2.71 2.49 2.43 2.42 2.39 2.30 2.28 2.11 2.09 0.80 0.54 0.50 0.49 0.45 0.44 0.44 0.42 0.42 0.41 0.41 0.40 0.37 0.37 0.30 0.27 0.16 0.15 0.15

0.79 0.73 0.61 0.58 0.56 0.55 0.55 0.53 0.50 0.48 0.47 0.45 0.45 0.43 0.43 0.40 0.39 0.38 0.38 0.36 0.36 0.32 0.32 -0.10 -0.27 -0.30 -0.31 -0.34 -0.36 -0.36 -0.38 -0.38 -0.39 -0.39 -0.39 -0.43 -0.44 -0.52 -0.56 -0.80 -0.82 -0.84

15:15 15:15 10:11 15:15 2:2 15:15 15:15 15:15 15:15 15:15 15:15 15:15 12:10 15:15 5:4 3:2 15:15 15:15 15:15 15:15 15:15 15:15 15:15 15:15 15:15 13:13 7:6 15:15 8:9 15:15 15:15 15:15 15:15 15:15 10:11 6:7 7:6 7:6 15:15 15:15 7:6 15:15

Journal of Proteome Research

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48

13 33

P23280 Q9UBC9

CAH6_HUMAN SPRR3_HUMAN

Carbonic anhydrase 6 OS=Homo sapiens GN=CA6 PE=1 SV=3 Small proline-rich protein 3 OS=Homo sapiens GN=SPRR3 PE=1 SV=2

Page 18 of 26

7.6E-04 8.3E-04

0.12 0.12

-0.91 -0.92

11:10 14:12

PS, pSS vs. SC pSS / SC pSS / SC pSS / SC pSS / SC ttest fold lin fold log n1-n2

Master N

Accession Number

Gene Name

Protein Name

17 140 26 94 25 13 15 29 97 28 6 42 163 209 61 92 76 1 128 182

P01857 P01859 P10909-2 P01764 P01877 P23280 P02787 P15515 P61769 P06870 P02788 Q08380 Q15782 Q9H0X9 P80188 P07476 P01609 P04745 P63104 P27487

IGHG1_HUMAN IGHG2_HUMAN CLUS_HUMAN HV303_HUMAN IGHA2_HUMAN CAH6_HUMAN TRFE_HUMAN HIS1_HUMAN B2MG_HUMAN KLK1_HUMAN TRFL_HUMAN LG3BP_HUMAN CH3L2_HUMAN OSBL5_HUMAN NGAL_HUMAN INVO_HUMAN KV117_HUMAN AMY1_HUMAN 1433Z_HUMAN DPP4_HUMAN

Ig gamma-1 chain C region OS=Homo sapiens GN=IGHG1 PE=1 SV=1 Ig gamma-2 chain C region OS=Homo sapiens GN=IGHG2 PE=1 SV=2 Isoform 2 of Clusterin OS=Homo sapiens GN=CLU Ig heavy chain V-III region VH26 OS=Homo sapiens PE=1 SV=1 Ig alpha-2 chain C region OS=Homo sapiens GN=IGHA2 PE=1 SV=3 Carbonic anhydrase 6 OS=Homo sapiens GN=CA6 PE=1 SV=3 Serotransferrin OS=Homo sapiens GN=TF PE=1 SV=3 Histatin-1 OS=Homo sapiens GN=HTN1 PE=1 SV=2 Beta-2-microglobulin OS=Homo sapiens GN=B2M PE=1 SV=1 Kallikrein-1 OS=Homo sapiens GN=KLK1 PE=1 SV=2 Lactotransferrin OS=Homo sapiens GN=LTF PE=1 SV=6 Galectin-3-binding protein OS=Homo sapiens GN=LGALS3BP PE=1 SV=1 Chitinase-3-like protein 2 OS=Homo sapiens GN=CHI3L2 PE=1 SV=1 Oxysterol-binding protein-related protein 5 OS=Homo sapiens GN=OSBPL5 PE=1 SV=1 Neutrophil gelatinase-associated lipocalin OS=Homo sapiens GN=LCN2 PE=1 SV=2 Involucrin OS=Homo sapiens GN=IVL PE=1 SV=2 Ig kappa chain V-I region Scw OS=Homo sapiens PE=1 SV=1 Alpha-amylase 1 OS=Homo sapiens GN=AMY1A PE=1 SV=2 14-3-3 protein zeta/delta OS=Homo sapiens GN=YWHAZ PE=1 SV=1 Dipeptidyl peptidase 4 OS=Homo sapiens GN=DPP4 PE=1 SV=2

1.6E-04 1.2E-03 2.7E-03 3.9E-03 9.1E-03 1.1E-02 1.4E-02 1.5E-02 1.5E-02 1.6E-02 2.1E-02 2.3E-02 2.7E-02 3.1E-02 3.2E-02 3.4E-02 3.4E-02 3.6E-02 3.6E-02 3.8E-02

Master N

Accession Number

Gene Name

Protein Name

SC / HC ttest

24 74 27 115 5

P0CG05 B9A064 Q96DR5 P04208 P01833

LAC2_HUMAN IGLL5_HUMAN BPIA2_HUMAN LV106_HUMAN PIGR_HUMAN

9.49 6.11 2.45 0.45 0.33 0.26 2.42 0.26 2.13 0.24 1.74 1.67 5.69 0.57 2.40 4.29 0.37 0.85 4.16 0.36

0.98 0.79 0.39 -0.34 -0.48 -0.59 0.38 -0.58 0.33 -0.63 0.24 0.22 0.76 -0.24 0.38 0.63 -0.43 -0.07 0.62 -0.44

15:14 15:14 15:14 15:14 15:14 11:10 15:14 15:14 10:10 15:14 15:14 15:14 5:3 8:5 15:14 8:5 8:8 15:14 5:3 8:9

PS, SC vs. HC

Ig lambda-2 chain C regions OS=Homo sapiens GN=IGLC2 PE=1 SV=1 Immunoglobulin lambda-like polypeptide 5 OS=Homo sapiens GN=IGLL5 PE=2 SV=2 BPI fold-containing family A member 2 OS=Homo sapiens GN=BPIFA2 PE=1 SV=2 Ig lambda chain V-I region WAH OS=Homo sapiens PE=1 SV=1 Polymeric immunoglobulin receptor OS=Homo sapiens GN=PIGR PE=1 SV=4

ACS Paragon Plus Environment

3.4E-06 6.5E-04 1.3E-03 1.9E-03 2.5E-03

SC / HC SC / HC fold lin fold log 4.69 3.32 0.28 4.00 2.93

0.67 0.52 -0.56 0.60 0.47

SC / HC n1-n2 14:15 14:15 14:15 14:15 14:15

Page 19 of 26

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Journal of Proteome Research

30 55 13 77 188 79 18 92 68 20 62 75 230 28 10 67 48 12 176 42 70 191

P01591 P04080 P23280 P52209 P01036 P08123 P01834 P07476 P06309 P01871 P07237 P05109 P07737 P06870 P22079 Q14508 P80303 P25311 Q6Q759 Q08380 P01743 P01700

IGJ_HUMAN CYTB_HUMAN CAH6_HUMAN 6PGD_HUMAN CYTS_HUMAN CO1A2_HUMAN IGKC_HUMAN INVO_HUMAN KV205_HUMAN IGHM_HUMAN PDIA1_HUMAN S10A8_HUMAN PROF1_HUMAN KLK1_HUMAN PERL_HUMAN WFDC2_HUMAN NUCB2_HUMAN ZA2G_HUMAN SPG17_HUMAN LG3BP_HUMAN HV102_HUMAN LV102_HUMAN

Immunoglobulin J chain OS=Homo sapiens GN=IGJ PE=1 SV=4 Cystatin-B OS=Homo sapiens GN=CSTB PE=1 SV=2 Carbonic anhydrase 6 OS=Homo sapiens GN=CA6 PE=1 SV=3 6-phosphogluconate dehydrogenase, decarboxylating OS=Homo sapiens GN=PGD PE=1 SV=3 Cystatin-S OS=Homo sapiens GN=CST4 PE=1 SV=3 Collagen alpha-2(I) chain OS=Homo sapiens GN=COL1A2 PE=1 SV=7 Ig kappa chain C region OS=Homo sapiens GN=IGKC PE=1 SV=1 Involucrin OS=Homo sapiens GN=IVL PE=1 SV=2 Ig kappa chain V-II region GM607 (Fragment) OS=Homo sapiens PE=4 SV=1 Ig mu chain C region OS=Homo sapiens GN=IGHM PE=1 SV=3 Protein disulfide-isomerase OS=Homo sapiens GN=P4HB PE=1 SV=3 Protein S100-A8 OS=Homo sapiens GN=S100A8 PE=1 SV=1 Profilin-1 OS=Homo sapiens GN=PFN1 PE=1 SV=2 Kallikrein-1 OS=Homo sapiens GN=KLK1 PE=1 SV=2 Lactoperoxidase OS=Homo sapiens GN=LPO PE=1 SV=2 WAP four-disulfide core domain protein 2 OS=Homo sapiens GN=WFDC2 PE=1 SV=2 Nucleobindin-2 OS=Homo sapiens GN=NUCB2 PE=1 SV=2 Zinc-alpha-2-glycoprotein OS=Homo sapiens GN=AZGP1 PE=1 SV=2 Sperm-associated antigen 17 OS=Homo sapiens GN=SPAG17 PE=1 SV=1 Galectin-3-binding protein OS=Homo sapiens GN=LGALS3BP PE=1 SV=1 Ig heavy chain V-I region HG3 OS=Homo sapiens PE=4 SV=1 Ig lambda chain V-I region HA OS=Homo sapiens PE=1 SV=1

Master N

Accession Number

Gene Name

Protein Name

56 1 30 142 82 53 139 156 67 31 161 207 58 12 51

Q8TDL5 Q9HC84 Q8N4F0 P80303 Q5QNW6 Q96DR5 P0CG05 P05204 P23280-2 P31025 Q8NBJ4 P68871 P63104 P13646 P15515

BPIB1_HUMAN MUC5B_HUMAN BPIB2_HUMAN NUCB2_HUMAN H2B2F_HUMAN BPIA2_HUMAN LAC2_HUMAN HMGN2_HUMAN CAH6_HUMAN LCN1_HUMAN GOLM1_HUMAN HBB_HUMAN 1433Z_HUMAN K1C13_HUMAN HIS1_HUMAN

BPI fold-containing family B member 1 OS=Homo sapiens GN=BPIFB1 PE=2 SV=1 Mucin-5B OS=Homo sapiens GN=MUC5B PE=1 SV=3 BPI fold-containing family B member 2 OS=Homo sapiens GN=BPIFB2 PE=1 SV=2 Nucleobindin-2 OS=Homo sapiens GN=NUCB2 PE=1 SV=2 Histone H2B type 2-F OS=Homo sapiens GN=HIST2H2BF PE=1 SV=3 BPI fold-containing family A member 2 OS=Homo sapiens GN=BPIFA2 PE=1 SV=2 Ig lambda-2 chain C regions OS=Homo sapiens GN=IGLC2 PE=1 SV=1 Non-histone chromosomal protein HMG-17 OS=Homo sapiens GN=HMGN2 PE=1 SV=3 Isoform 2 of Carbonic anhydrase 6 OS=Homo sapiens GN=CA6 Lipocalin-1 OS=Homo sapiens GN=LCN1 PE=1 SV=1 Golgi membrane protein 1 OS=Homo sapiens GN=GOLM1 PE=1 SV=1 Hemoglobin subunit beta OS=Homo sapiens GN=HBB PE=1 SV=2 14-3-3 protein zeta/delta OS=Homo sapiens GN=YWHAZ PE=1 SV=1 Keratin, type I cytoskeletal 13 OS=Homo sapiens GN=KRT13 PE=1 SV=4 Histatin-1 OS=Homo sapiens GN=HTN1 PE=1 SV=2

2.5E-03 4.4E-03 9.2E-03 1.2E-02 1.4E-02 1.4E-02 1.5E-02 1.8E-02 1.8E-02 2.2E-02 2.2E-02 2.2E-02 2.2E-02 2.2E-02 2.5E-02 2.6E-02 2.7E-02 3.1E-02 3.4E-02 3.8E-02 4.0E-02 4.2E-02

2.45 0.22 0.48 0.41 0.04 0.37 2.75 0.12 2.05 2.37 0.53 0.30 0.51 2.81 0.55 2.16 0.51 1.71 0.58 1.68 2.63 3.22

0.39 -0.66 -0.31 -0.39 -1.37 -0.43 0.44 -0.90 0.31 0.37 -0.28 -0.53 -0.30 0.45 -0.26 0.33 -0.30 0.23 -0.24 0.22 0.42 0.51

WS, pSS vs. HC

ACS Paragon Plus Environment

pSS / HC pSS / HC pSS / HC pSS / HC ttest fold lin fold log n1-n2 1.2E-05 1.3E-05 2.9E-05 4.8E-04 6.3E-04 7.7E-04 1.0E-03 1.1E-03 1.1E-03 1.4E-03 2.7E-03 2.9E-03 3.5E-03 4.0E-03 4.5E-03

0.07 0.12 0.10 0.13 6.76 0.11 3.96 2.74 0.13 0.22 0.26 0.14 0.40 5.38 0.16

-1.15 -0.92 -1.02 -0.90 0.83 -0.95 0.60 0.44 -0.89 -0.66 -0.58 -0.86 -0.40 0.73 -0.79

11:11 15:15 11:11 5:5 13:13 15:15 15:15 9:9 11:11 15:15 9:9 11:11 15:15 13:13 15:15

14:15 14:15 10:10 5:6 2:2 6:7 14:15 5:6 14:15 14:15 10:11 14:15 3:4 14:15 14:15 14:15 14:15 14:15 2:2 14:15 12:13 2:2

Journal of Proteome Research

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48

238 81 323 3 32 115 35 14 50 100 16 180 10 2 134 116 258 270 38 68 181 22 123 294 244 296 24 312 110 49 119 173 190 42

P0CF74 P52209 P22392-2 P04745 P04083 P62805 B9A064 Q9UGM3-5 P18136 P09228 P01834 Q6FI13 P02538 P02810 P28325 P01009 P55058 P59998 P12273 P54108 P16401 P01857 P04792 P81605 Q92876 P11684 P01591 P01621 P02675 Q9UBG3 Q71DI3 P04259 P06703 P01877

LAC6_HUMAN 6PGD_HUMAN NDKB_HUMAN AMY1_HUMAN ANXA1_HUMAN H4_HUMAN IGLL5_HUMAN DMBT1_HUMAN KV313_HUMAN CYTT_HUMAN IGKC_HUMAN H2A2A_HUMAN K2C6A_HUMAN PRPC_HUMAN CYTD_HUMAN A1AT_HUMAN PLTP_HUMAN ARPC4_HUMAN PIP_HUMAN CRIS3_HUMAN H15_HUMAN IGHG1_HUMAN HSPB1_HUMAN DCD_HUMAN KLK6_HUMAN UTER_HUMAN IGJ_HUMAN KV303_HUMAN FIBB_HUMAN CRNN_HUMAN H32_HUMAN K2C6B_HUMAN S10A6_HUMAN IGHA2_HUMAN

Master N

Accession Number

Gene Name

67 51 53

P23280-2 P15515 Q96DR5

CAH6_HUMAN HIS1_HUMAN BPIA2_HUMAN

Page 20 of 26

Ig lambda-6 chain C region OS=Homo sapiens GN=IGLC6 PE=4 SV=1 5.4E-03 6-phosphogluconate dehydrogenase, decarboxylating OS=Homo sapiens GN=PGD PE=1 SV=3 6.1E-03 Isoform 3 of Nucleoside diphosphate kinase B OS=Homo sapiens GN=NME2 8.2E-03 Alpha-amylase 1 OS=Homo sapiens GN=AMY1A PE=1 SV=2 1.1E-02 Annexin A1 OS=Homo sapiens GN=ANXA1 PE=1 SV=2 1.1E-02 Histone H4 OS=Homo sapiens GN=HIST1H4A PE=1 SV=2 1.1E-02 Immunoglobulin lambda-like polypeptide 5 OS=Homo sapiens GN=IGLL5 PE=2 SV=2 1.2E-02 Isoform 5 of Deleted in malignant brain tumors 1 protein OS=Homo sapiens GN=DMBT1 1.4E-02 Ig kappa chain V-III region HIC OS=Homo sapiens PE=2 SV=2 1.4E-02 Cystatin-SA OS=Homo sapiens GN=CST2 PE=1 SV=1 1.6E-02 Ig kappa chain C region OS=Homo sapiens GN=IGKC PE=1 SV=1 1.8E-02 Histone H2A type 2-A OS=Homo sapiens GN=HIST2H2AA3 PE=1 SV=3 1.8E-02 Keratin, type II cytoskeletal 6A OS=Homo sapiens GN=KRT6A PE=1 SV=3 2.1E-02 Salivary acidic proline-rich phosphoprotein 1/2 OS=Homo sapiens GN=PRH1 PE=1 SV=2 2.5E-02 Cystatin-D OS=Homo sapiens GN=CST5 PE=1 SV=1 2.6E-02 Alpha-1-antitrypsin OS=Homo sapiens GN=SERPINA1 PE=1 SV=3 2.6E-02 Phospholipid transfer protein OS=Homo sapiens GN=PLTP PE=1 SV=1 2.8E-02 Actin-related protein 2/3 complex subunit 4 OS=Homo sapiens GN=ARPC4 PE=1 SV=3 2.9E-02 Prolactin-inducible protein OS=Homo sapiens GN=PIP PE=1 SV=1 3.0E-02 Cysteine-rich secretory protein 3 OS=Homo sapiens GN=CRISP3 PE=1 SV=1 3.0E-02 Histone H1.5 OS=Homo sapiens GN=HIST1H1B PE=1 SV=3 3.1E-02 Ig gamma-1 chain C region OS=Homo sapiens GN=IGHG1 PE=1 SV=1 3.2E-02 Heat shock protein beta-1 OS=Homo sapiens GN=HSPB1 PE=1 SV=2 3.7E-02 Dermcidin OS=Homo sapiens GN=DCD PE=1 SV=2 3.7E-02 Kallikrein-6 OS=Homo sapiens GN=KLK6 PE=1 SV=1 3.8E-02 Uteroglobin OS=Homo sapiens GN=SCGB1A1 PE=1 SV=1 3.8E-02 Immunoglobulin J chain OS=Homo sapiens GN=IGJ PE=1 SV=4 3.8E-02 Ig kappa chain V-III region NG9 (Fragment) OS=Homo sapiens PE=1 SV=1 4.0E-02 Fibrinogen beta chain OS=Homo sapiens GN=FGB PE=1 SV=2 4.1E-02 Cornulin OS=Homo sapiens GN=CRNN PE=1 SV=1 4.1E-02 Histone H3.2 OS=Homo sapiens GN=HIST2H3A PE=1 SV=3 4.3E-02 Keratin, type II cytoskeletal 6B OS=Homo sapiens GN=KRT6B PE=1 SV=5 4.6E-02 Protein S100-A6 OS=Homo sapiens GN=S100A6 PE=1 SV=1 4.6E-02 Ig alpha-2 chain C region OS=Homo sapiens GN=IGHA2 PE=1 SV=3 4.6E-02

3.59 0.37 0.95 0.27 3.67 9.26 2.97 0.36 2.44 0.27 2.53 8.37 3.99 0.08 0.35 0.38 0.51 1.72 0.32 0.43 3.56 2.84 2.19 0.31 2.74 0.30 2.19 2.21 0.65 0.41 4.11 6.16 0.55 0.34

0.56 -0.43 -0.02 -0.56 0.57 0.97 0.47 -0.44 0.39 -0.57 0.40 0.92 0.60 -1.07 -0.46 -0.42 -0.30 0.24 -0.50 -0.37 0.55 0.45 0.34 -0.51 0.44 -0.52 0.34 0.34 -0.19 -0.39 0.61 0.79 -0.26 -0.47

11:11 11:11 2:2 15:15 11:11 3:3 9:9 15:15 13:13 9:9 15:15 3:3 11:11 3:3 11:11 11:11 9:9 3:3 15:15 15:15 7:7 13:13 7:7 2:2 4:4 6:6 15:15 11:11 11:11 13:13 11:11 8:8 15:15 11:11

WS, pSS vs. SC Protein Name Isoform 2 of Carbonic anhydrase 6 OS=Homo sapiens GN=CA6 Histatin-1 OS=Homo sapiens GN=HTN1 PE=1 SV=2 BPI fold-containing family A member 2 OS=Homo sapiens GN=BPIFA2 PE=1 SV=2

ACS Paragon Plus Environment

pSS / SC pSS / SC pSS / SC pSS / SC ttest fold lin fold log n1-n2 4.8E-04 5.2E-04 3.4E-03

0.13 0.12 0.14

-0.88 -0.93 -0.85

11:11 15:15 15:15

Page 21 of 26

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48

Journal of Proteome Research

265 270 42 180 14 2 22 156 11 126 115 267 90 69 3 39 8 68

Q71U36 P59998 P01877 Q6FI13 Q9UGM3-5 P02810 P01857 P05204 P02814 P06870 P62805 Q92817 P31146 Q6P5S2 P04745 P05164 P02788 P54108

TBA1A_HUMAN ARPC4_HUMAN IGHA2_HUMAN H2A2A_HUMAN DMBT1_HUMAN PRPC_HUMAN IGHG1_HUMAN HMGN2_HUMAN SMR3B_HUMAN KLK1_HUMAN H4_HUMAN EVPL_HUMAN COR1A_HUMAN CF058_HUMAN AMY1_HUMAN PERM_HUMAN TRFL_HUMAN CRIS3_HUMAN

Master N

Accession Number

Gene Name

1 56 30 31 161 58 18 207 48 240 12 81 4 140 32 11 153

Q9HC84 Q8TDL5 Q8N4F0 P31025 Q8NBJ4 P63104 P04406 P68871 P14618 Q9NSB4 P13646 P52209 P02768 P23284 P04083 P02814 P69905

MUC5B_HUMAN BPIB1_HUMAN BPIB2_HUMAN LCN1_HUMAN GOLM1_HUMAN 1433Z_HUMAN G3P_HUMAN HBB_HUMAN KPYM_HUMAN KRT82_HUMAN K1C13_HUMAN 6PGD_HUMAN ALBU_HUMAN PPIB_HUMAN ANXA1_HUMAN SMR3B_HUMAN HBA_HUMAN

Tubulin alpha-1A chain OS=Homo sapiens GN=TUBA1A PE=1 SV=1 3.4E-03 Actin-related protein 2/3 complex subunit 4 OS=Homo sapiens GN=ARPC4 PE=1 SV=3 5.0E-03 Ig alpha-2 chain C region OS=Homo sapiens GN=IGHA2 PE=1 SV=3 5.3E-03 Histone H2A type 2-A OS=Homo sapiens GN=HIST2H2AA3 PE=1 SV=3 8.0E-03 Isoform 5 of Deleted in malignant brain tumors 1 protein OS=Homo sapiens GN=DMBT1 9.7E-03 Salivary acidic proline-rich phosphoprotein 1/2 OS=Homo sapiens GN=PRH1 PE=1 SV=2 1.1E-02 Ig gamma-1 chain C region OS=Homo sapiens GN=IGHG1 PE=1 SV=1 1.2E-02 Non-histone chromosomal protein HMG-17 OS=Homo sapiens GN=HMGN2 PE=1 SV=3 1.4E-02 Submaxillary gland androgen-regulated protein 3B OS=Homo sapiens GN=SMR3B PE=1 SV=2 1.5E-02 Kallikrein-1 OS=Homo sapiens GN=KLK1 PE=1 SV=2 1.9E-02 Histone H4 OS=Homo sapiens GN=HIST1H4A PE=1 SV=2 2.4E-02 Envoplakin OS=Homo sapiens GN=EVPL PE=1 SV=3 2.6E-02 Coronin-1A OS=Homo sapiens GN=CORO1A PE=1 SV=4 2.6E-02 UPF0762 protein C6orf58 OS=Homo sapiens GN=C6orf58 PE=1 SV=2 2.7E-02 Alpha-amylase 1 OS=Homo sapiens GN=AMY1A PE=1 SV=2 3.5E-02 Myeloperoxidase OS=Homo sapiens GN=MPO PE=1 SV=1 3.5E-02 Lactotransferrin OS=Homo sapiens GN=LTF PE=1 SV=6 4.2E-02 Cysteine-rich secretory protein 3 OS=Homo sapiens GN=CRISP3 PE=1 SV=1 4.3E-02

3.31 2.64 0.23 10.09 0.34 0.03 3.29 2.33 0.05 0.25 6.73 7.91 2.01 0.38 0.36 3.41 2.77 0.44

0.52 0.42 -0.64 1.00 -0.47 -1.59 0.52 0.37 -1.30 -0.60 0.83 0.90 0.30 -0.42 -0.44 0.53 0.44 -0.35

2:2 3:3 11:11 3:3 15:15 3:3 13:13 9:9 5:5 13:13 3:3 2:2 13:13 15:15 15:15 13:13 15:15 15:15

WS, SC vs. HC Protein Name

SC / HC ttest

Mucin-5B OS=Homo sapiens GN=MUC5B PE=1 SV=3 5.3E-09 BPI fold-containing family B member 1 OS=Homo sapiens GN=BPIFB1 PE=2 SV=1 4.2E-06 BPI fold-containing family B member 2 OS=Homo sapiens GN=BPIFB2 PE=1 SV=2 2.6E-05 Lipocalin-1 OS=Homo sapiens GN=LCN1 PE=1 SV=1 1.2E-04 Golgi membrane protein 1 OS=Homo sapiens GN=GOLM1 PE=1 SV=1 2.4E-04 14-3-3 protein zeta/delta OS=Homo sapiens GN=YWHAZ PE=1 SV=1 2.5E-03 Glyceraldehyde-3-phosphate dehydrogenase OS=Homo sapiens GN=GAPDH PE=1 SV=3 2.5E-03 Hemoglobin subunit beta OS=Homo sapiens GN=HBB PE=1 SV=2 5.0E-03 Pyruvate kinase PKM OS=Homo sapiens GN=PKM PE=1 SV=4 5.8E-03 Keratin, type II cuticular Hb2 OS=Homo sapiens GN=KRT82 PE=1 SV=3 1.2E-02 Keratin, type I cytoskeletal 13 OS=Homo sapiens GN=KRT13 PE=1 SV=4 1.2E-02 6-phosphogluconate dehydrogenase, decarboxylating OS=Homo sapiens GN=PGD PE=1 SV=3 1.3E-02 Serum albumin OS=Homo sapiens GN=ALB PE=1 SV=2 1.3E-02 Peptidyl-prolyl cis-trans isomerase B OS=Homo sapiens GN=PPIB PE=1 SV=2 1.8E-02 Annexin A1 OS=Homo sapiens GN=ANXA1 PE=1 SV=2 2.7E-02 Submaxillary gland androgen-regulated protein 3B OS=Homo sapiens GN=SMR3B PE=1 SV=2 3.1E-02 Hemoglobin subunit alpha OS=Homo sapiens GN=HBA1 PE=1 SV=2 4.4E-02

ACS Paragon Plus Environment

SC / HC SC / HC fold lin fold log 0.07 0.06 0.16 0.13 0.22 0.42 0.40 0.13 0.28 0.10 3.94 0.44 0.41 0.46 2.18 6.92 0.21

-1.15 -1.25 -0.80 -0.90 -0.66 -0.37 -0.39 -0.89 -0.56 -1.01 0.60 -0.35 -0.39 -0.34 0.34 0.84 -0.69

SC / HC n1-n2 15:15 11:11 11:11 15:15 9:9 15:15 13:13 11:11 13:13 2:2 13:13 11:11 15:15 13:13 11:11 5:5 9:9

Journal of Proteome Research

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 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 60

Page 22 of 26

Table S-3. WGA lectin affinity capture and MS identification of glycoproteins and N-glycosites from pSS, SC, and HC whole saliva samples. pSS Accession Number

Protein

Glycosite

Sequence*

P00738

Haptoglobin

HPT_HUMAN@184 HPT_HUMAN@241

MVSHHNLTTGATLINEQWLLTTAK VVLHPNYSQVDIGLIK

x x

P01833

Polymeric immunoglobulin receptor

PIGR_HUMAN@135 PIGR_HUMAN@186 PIGR_HUMAN@469 PIGR_HUMAN@83

GLSFDVSLEVSQGPGLLNDTK GLYPVLVIDSSGYVNPNYTGR VPGNVTAVLGETLK ANLTNFPENGTFVVNIAQLSQDDSGR

x x x x

P01871

Ig mu chain C region

IGHM_HUMAN@209 IGHM_HUMAN@439

GLTFQQNASSMCVPDQDTAIR STGKPTLYNVSLVMSDTAGTCY

x x

P01876

Ig alpha-1 chain C region

IGHA1_HUMAN@144 IGHA1_HUMAN@340

GSEANLTCTLTGLR LAGKPTHVNVSVVMAEVDGTCY

P01877

Ig alpha-2 chain C region

IGHA2_HUMAN@131 IGHA2_HUMAN@327 IGHA2_HUMAN@47

P02788

Lactotransferrin

SC

HC x

x x x x

x x x x

x x

x x

x x

ALEDLLLGSEANLTCTLTGLR PTHVNVSVVMAEVDGTCY QGFFPQEPLSVTWSESGQNVTAR

x x x

x x x

x

TRFL_HUMAN@156 TRFL_HUMAN@497

PFLNWTGPPEPIEAAVAR TAGWNIPMGLLFNQTGSCK

x x

x x

P02790

Hemopexin

HEMO_HUMAN@453

ALPQPQNVTSLLGCTH

x

P80188

Neutrophil gelatinase-associated lipocalin

NGAL_HUMAN@85

SYNVTSVLFR

x

Q02413

Desmoglein-1

DSG1_HUMAN@110

TGEINITSIVDR

x

Q08380

Galectin-3-binding protein

LG3BP_HUMAN@69

ALGFENATQALGR

x

P80188

Neutrophil gelatinase-associated lipocalin

NGAL_HUMAN@85

SYNVTSVLFR

x

Q08380

Galectin-3-binding protein

LG3BP_HUMAN@69

ALGFENATQALGR

x

Q9HC84

Mucin-5B

MUC5B_HUMAN@1556 MUC5B_HUMAN@254 MUC5B_HUMAN@4960 MUC5B_HUMAN@5046 MUC5B_HUMAN@805 MUC5B_HUMAN@929 MUC5B_HUMAN@1244 MUC5B_HUMAN@5017 MUC5B_HUMAN@5024 MUC5B_HUMAN@5111

DIECQAESFPNWTLAQVGQK LDGPTEQCPDPLPLPAGNCTDEEGICHR AFGQFFSPGEVIYNK(T) VVLLDPKPVANVTCVNK STGCAAPMVYLDCSNSSAGTPGAECLR YSFEGSCEYILAQDYCGDNTTHGTFR VPTAENCQSCNCTPSGIQCAHSLEACTCTYEDR QVNETWTLENCTVAR QVNETWTLENCTVAR FGNLSLYLDNHYCTASATAAAAR

x x x x x x

x x x x x

Q9UGM3

Deleted in malignant brain tumors 1

DMBT1_HUMAN@1889

LVNLNSSYGLCAGR

x

x

* The consensus sequence is highlighted in red.

ACS Paragon Plus Environment

x x x

x

x x x x x x x x x x

Page 23 of 26

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 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 60

Journal of Proteome Research

Table S-4. AAL lectin affinity capture and MS identification of glycoproteins and N-glycosites from pSS, SC, and HC parotid saliva samples. pSS

SC

HC

GLSFDVSLEVSQGPGLLNDTK LVIDSSGYVNPNYTGR VPGNVTAVLGETLK ANLTNFPENGTFVVNIAQLSQDDSGR

x x x x

x x x x

x x x x

Accession Number

Protein

Glycosite

Sequence*

P01833

Polymeric immunoglobulin receptor

PIGR_HUMAN@135 PIGR_HUMAN@186 PIGR_HUMAN@469 PIGR_HUMAN@83

P01876

Ig alpha-1 chain C region

IGHA1_HUMAN@144 IGHA1_HUMAN@340

HRPALEDLLLGSEANLTCTLTGLR LAGKPTHVNVSVVMAEVDGTCY

x x

x x

P01877

Ig alpha-2 chain C region

IGHA2_HUMAN@131 IGHA2_HUMAN@327 IGHA2_HUMAN@47

HRPALEDLLLGSEANLTCTLTGLR AGKPTHVNVSVVMAEVDGTCY QGFFPQEPLSVTWSESGQNVTAR

x x x

x x

P02788

Lactotransferrin

TRFL_HUMAN@156 TRFL_HUMAN@497

LNWTGPPEPIEAAVAR TAGWNIPMGLLFNQTGSCK

x x

P04220

Ig mu heavy chain disease protein

MUCB_HUMAN@378

STGKPTLYNVSLVMSDTAGTCY

x

P22079

Lactoperoxidase

PERL_HUMAN@106 PERL_HUMAN@212

ASLTNVTDPSLDLTSLSLEVGCGAPAPVVR IVGYLNEEGVLDQNR(S)

x x

x x

P25311

Zinc-alpha-2-glycoprotein

ZA2G_HUMAN@109

DIVEYYNDSNGSHVLQGR

x

x

Q08380

Galectin-3-binding protein

LG3BP_HUMAN@69

ALGFENATQALGR

x

P04745

Alpha-amylase 1

AMY1_HUMAN@476

INGNCTGIK

* The consensus sequence is highlighted in red.

ACS Paragon Plus Environment

x

Journal of Proteome Research

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 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 60

Page 24 of 26

Table S-5. AAL lectin affinity capture and MS identification of glycoproteins and N-glycosites from pSS, SC, and HC whole saliva samples. pSS

SC

Accession Number

Protein

Glycosite

Sequence*

P00738

Haptoglobin

HPT_HUMAN@184 HPT_HUMAN@241

MVSHHNLTTGATLINEQWLLTTAK VVLHPNYSQVDIGLIK

x x

P01033

Metalloproteinase inhibitor 1

TIMP1_HUMAN@53

FVGTPEVNQTTLYQR

x

x

P01833

Polymeric immunoglobulin receptor

PIGR_HUMAN@135 PIGR_HUMAN@186 PIGR_HUMAN@469 PIGR_HUMAN@83

GLSFDVSLEVSQGPGLLNDTK LVIDSSGYVNPNYTGR VPGNVTAVLGETLK ANLTNFPENGTFVVNIAQLSQDDSGR

x x x x

x x x x

HC

x x x

P01871

Ig mu chain C region

IGHM_HUMAN@209

GLTFQQNASSMCVPDQDTAIR

x

x

P01876

Ig alpha-1 chain C region

IGHA1_HUMAN@144 IGHA1_HUMAN@340

ALEDLLLGSEANLTCTLTGLR LAGKPTHVNVSVVMAEVDGTCY

x x

x x

x x

P01877

Ig alpha-2 chain C region

IGHA2_HUMAN@131 IGHA2_HUMAN@327 IGHA2_HUMAN@47

ALEDLLLGSEANLTCTLTGLR PTHVNVSVVMAEVDGTCY QGFFPQEPLSVTWSESGQNVTAR

x x x

x x x

x x x

P02787

Serotransferrin

TRFE_HUMAN@630

QQQHLFGSNVTDCSGNFCLFR

x

x

P02788

Lactotransferrin

TRFL_HUMAN@156 TRFL_HUMAN@497

PFLNWTGPPEPIEAAVAR TAGWNIPMGLLFNQTGSCK

x x

x

x x

P02790

Hemopexin

HEMO_HUMAN@453

ALPQPQNVTSLLGCTH

x

P05164

Myeloperoxidase

PERM_HUMAN@729

DFVNCSTLPALNLASWR

x

x

P10909

Clusterin

CLUS_HUMAN@374

LANLTQGEDQYYLR

x

x

P13646

Keratin, type I cytoskeletal 13

K1C13_HUMAN@446

STSVTTTSSASVTTTSNASGR

x

x

P20061

Transcobalamin-1

TCO1_HUMAN@369

MNDTIFGFTMEER

x

x

P22079

Lactoperoxidase

PERL_HUMAN@212 PERL_HUMAN@322

IVGYLNEEGVLDQNR(S) NLSSPLGLMAVNQEVSDHGLPYLPYDSK

x

x x

P25311

Zinc-alpha-2-glycoprotein

ZA2G_HUMAN@109

DIVEYYNDSNGSHVLQGR

x

x

P32926

Desmoglein-3

DSG3_HUMAN@110

TGEINITSIVDR

x

P80188

Neutrophil gelatinase-associated lipocalin

NGAL_HUMAN@85

SYNVTSVLFR

x

Q02413

Desmoglein-1

DSG1_HUMAN@110

TGEINITSIVDR

x

Q02487

Desmocollin-2

DSC2_HUMAN@546

NGIYNITVLASDQGGR

x

Q08380

Galectin-3-binding protein

LG3BP_HUMAN@69

ALGFENATQALGR

x

P80188

Neutrophil gelatinase-associated lipocalin

NGAL_HUMAN@85

SYNVTSVLFR

x

Q08380

Galectin-3-binding protein

LG3BP_HUMAN@69

ALGFENATQALGR

x

x

Q9HC84

Mucin-5B

MUC5B_HUMAN@1556 MUC5B_HUMAN@254 MUC5B_HUMAN@4960 MUC5B_HUMAN@5017 MUC5B_HUMAN@5024 MUC5B_HUMAN@5046 MUC5B_HUMAN@805 MUC5B_HUMAN@929

DIECQAESFPNWTLAQVGQK LDGPTEQCPDPLPLPAGNCTDEEGICHR AFGQFFSPGEVIYNK(T) QVNETWTLENCTVAR QVNETWTLENCTVAR VVLLDPKPVANVTCVNK STGCAAPMVYLDCSNSSAGTPGAECLR YSFEGSCEYILAQDYCGDNTTHGTFR

x x x x x x x x

x x x

x x x

x x

x x x x

x

x

Q9UGM3

Deleted in malignant brain tumors 1

DMBT1_HUMAN@1889

LVNLNSSYGLCAGR

x

x

Q9Y6R7

IgGFc-binding protein

FCGBP_HUMAN@5186 FCGBP_HUMAN@91

YLPVNSSLLTSDCSER VTVRPGESVMVNISAK

x x

x

P06870

Kallikrein-1

KLK1_HUMAN@102 KLK1_HUMAN@108

Q8N4F0

BPI fold-containing family B member 2

BPIB2_HUMAN@293 BPIB2_HUMAN@332

HNLFDDENTAQFVHVSESFPHPGFNMSLLEN HTR HNLFDDENTAQFVHVSESFPHPGFNMSLLEN HTR SDDNLLNTSALGR LGATPVAMLHTNNATLR

* The consensus sequence is highlighted in red.

ACS Paragon Plus Environment

x x

x x x x

Page 25 of 26

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Journal of Proteome Research

Table S-6. Legend matching shapes to protein families for Figures 3a and 3b.

ACS Paragon Plus Environment

Journal of Proteome Research

For TOC Only

100

b2M

80

pSS

60

SC

40

HC

20 0

Relative Intensity

Percent of Total N-Glycosites

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48

Page 26 of 26

1.2 1 0.8 0.6 0.4 0.2 0 pSS

PS

WS

ACS Paragon Plus Environment

Healthy