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000276354 037__ $$aDKFZ-2023-01074
000276354 041__ $$aEnglish
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000276354 1001_ $$00000-0002-3761-6883$$aDriver, Taran$$b0
000276354 245__ $$aIdentification of Cofragmented Combinatorial Peptide Isomers by Two-Dimensional Partial Covariance Mass Spectrometry.
000276354 260__ $$aWashington, DC$$bACS Publications$$c2023
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000276354 500__ $$a2023 Jul 5;34(7):1230-1234
000276354 520__ $$aCombinatorial post-translational modifications (PTMs), such as those forming the so-called 'histone code', have been linked to cell differentiation, embryonic development, cellular reprogramming, aging, cancers, neurodegenerative disorders, etc. Nevertheless, a reliable mass spectral analysis of the combinatorial isomers represents a considerable challenge. The difficulty stems from the incompleteness of information that could be generated by the standard MS to differentiate cofragmented isomeric sequences in their naturally occurring mixtures based on the fragment mass-to-charge ratio and relative abundance information only. Here we show that fragment-fragment correlations revealed by two-dimensional partial covariance mass spectrometry (2D-PC-MS) allow one to solve the combinatorial PTM puzzles that cannot be tackled by the standard MS as a matter of principle. We introduce 2D-PC-MS marker ion correlation approach and demonstrate experimentally that it can provide the missing information enabling identification of cofragmentated combinatorially modified isomers. Our in silico study shows that the marker ion correlations can be used to unambiguously identify 5 times more cofragmented combinatorially acetylated tryptic peptides and 3 times more combinatorially modified Glu-C peptides of human histones than is possible using standard MS methods.
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000276354 650_7 $$2Other$$a2D-PC-MS
000276354 650_7 $$2Other$$acombinatorial PTMs
000276354 650_7 $$2Other$$ahistones
000276354 650_7 $$2Other$$amarker ion correlations
000276354 650_7 $$2Other$$amass spectrometry
000276354 7001_ $$0P:(DE-HGF)0$$aPipkorn, Rüdiger$$b1
000276354 7001_ $$00000-0001-7999-0075$$aAverbukh, Vitali$$b2
000276354 7001_ $$aFrasinski, Leszek J$$b3
000276354 7001_ $$aMarangos, Jon P$$b4
000276354 7001_ $$00000-0002-7288-375X$$aEdelson-Averbukh, Marina$$b5
000276354 773__ $$0PERI:(DE-600)2019911-9$$a10.1021/jasms.3c00111$$gp. jasms.3c00111$$n7$$p1230-1234$$tJournal of the American Society for Mass Spectrometry$$v34$$x1044-0305$$y2023
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