Rapid and selective screening for sulfhydryl analytes in plasma and urine using surface-enhanced transmission mode desorption electrospray ionization mass spectrometry.
Nylon mesh substrates were derivatized to include VICAT(SH), a biotinylated reagent that contains both a photolabile linking group and a thiol specific capture agent. The enhanced mesh substrates were then used to capture sulfhydryl analytes directly from urine and plasma samples via covalent reaction between the reactive thiols of the analytes and the iodoacetaminyl unit of VICAT(SH). Photocleavage of the labile linker was followed by direct analysis of the mesh surface via transmission mode desorption electrospray ionization (TM-DESI). This chemoselective capture method promoted enrichment of sulfhydryl analytes and reduced matrix interferences, thereby resulting in increased analytical performance of surface enhanced TM-DESI-MS when compared to standard DESI-MS. The present work describes the manufacture of the derivatized mesh substrates and the quality control assessments made during the manufacturing process, the optimization of the chemoselective capture method, and results of experiments pertinent to biological applications. Integration of the chemoselective capture materials with ambient ionization and tandem mass spectrometry results in a powerful combination of speed and selectivity for targeted analyte screening.
Chipuk
Joseph E
JE
Department of Chemistry and Biochemistry, University of Texas at Austin, University Station A5300, Austin, Texas 78712, USA.
Gelb
Michael H
MH
Brodbelt
Jennifer S
JS
D004364:Pharmaceutical Preparations / Q000737:chemistry*; D021241:Spectrometry, Mass, Electrospray Ionization / Q000379:methods*; D013438:Sulfhydryl Compounds / Q000737:chemistry*; D053719:Tandem Mass Spectrometry / Q000379:methods*
D004364:Pharmaceutical Preparations; D013438:Sulfhydryl Compounds
Anal Chem. 2007 Aug 1;79(15):5878-87
17602570
J Pharm Biomed Anal. 2009 Oct 15;50(3):384-91
19525082
Nat Methods. 2007 May;4(5):429-35
17417646
Nucleic Acids Res. 1999 Dec 1;27(23):4626-31
10556319
Anal Chem. 2007 Nov 1;79(21):8327-32
17918908
Anal Chem. 2009 Sep 15;81(18):7618-24
19746995
Proc Natl Acad Sci U S A. 1995 Aug 1;92(16):7590-4
7638235
J Chromatogr B Analyt Technol Biomed Life Sci. 2003 Nov 25;797(1-2):305-19
14630157
J Am Soc Mass Spectrom. 2009 Apr;20(4):584-92
19112027
Anal Chem. 2007 Mar 1;79(5):2150-7
17269655
J Am Chem Soc. 2007 Dec 26;129(51):15780-2
18052286
Nat Mater. 2008 Jun;7(6):442-53
18497851
J Chromatogr. 1991 Jan 2;562(1-2):639-45
2026726
Proteomics. 2009 Mar;9(6):1518-23
19294621
Bioconjug Chem. 2004 Mar-Apr;15(2):380-8
15025535
Proc Natl Acad Sci U S A. 1971 Sep;68(9):2153-7
5289374
Methods Enzymol. 2009;463:417-38
19892186
Mass Spectrom Rev. 1997 Nov-Dec;16(6):353-76
9703694
Mass Spectrom Rev. 2004 Jan-Feb;23(1):34-44
14625891
Anal Chem. 2010 Jan 1;82(1):16-8
19902914
Methods Mol Biol. 1995;42:1-218
7655571
Proc Natl Acad Sci U S A. 2003 Jan 21;100(2):409-13
12515854
J Am Soc Mass Spectrom. 2008 Nov;19(11):1612-20
18684639
Comp Biochem Physiol B Biochem Mol Biol. 2002 Dec;133(4):523-35
12470816
Rapid Commun Mass Spectrom. 1996;10(13):1688-92
8914339
Anal Chem. 2002 Mar 15;74(6):1349-54
11922303
Anal Chem. 1999 May 15;71(10):2014-20
10361500
Anal Bioanal Chem. 2006 Jul;385(5):855-60
16791565
J Agric Food Chem. 2008 Jan 23;56(2):333-6
18092755
Cancer Invest. 2007 Mar;25(2):117-23
17453823
Analyst. 2008 Nov;133(11):1481-5
18936823
J Mass Spectrom. 2005 Oct;40(10):1261-75
16237663
Br J Clin Pharmacol. 1984 Mar;17(3):243-50
6324834
ACS Nano. 2008 Jan;2(1):7-18
19206542
Science. 2004 Oct 15;306(5695):471-3
15486296
Science. 2006 Mar 17;311(5767):1566-70
16543450
Anal Chem. 2007 Sep 15;79(18):7131-8
17705399
Anal Chem. 2002 Jul 15;74(14):3429-33
12139050
Biomed Chromatogr. 2003 Jul;17(5):285-91
12884392
Enzyme Microb Technol. 2001 Feb 1;28(2-3):225-232
11166816
Anal Biochem. 2008 Apr 15;375(2):187-95
18162165
Anal Chem. 1995 Mar 1;67(5):843-8
7762820
Anal Bioanal Chem. 2005 Mar;381(5):1095-100
15744519
Anal Chem. 2004 Jul 15;76(14):4104-11
15253649
Anal Biochem. 1981 Apr;112(2):195-203
6266278
J Mol Biol. 1975 Nov 5;98(3):503-17
1195397
Anal Chem. 2005 Apr 15;77(8):2297-302
15828760