Peptide dimethylation: fragmentation control via distancing the dimethylamino group.
Peptide dimethylation: fragmentation control via distancing the dimethylamino group.
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DOI：
10.1007/s13361-014-0951-7
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发表时间：
2014-10
影响因子：
3.2
通讯作者：
Yao, Xudong
中科院分区：
文献类型：
--
作者：
McShane, Adam J.;Shen, Yuanyuan;Castillo, Mary Joan;Yao, Xudong
关键词：
肽的直接还原甲基化是定量蛋白质组学的常用方法。这是一种活性衍生化技术;在二甲氨基的参与下，衍生化肽优先释放强α 1离子。然而，用于定量蛋白质组学分析的α 1离子的有利产生对于使用多反应监测质谱的靶向蛋白质组学定量是不期望的;这种质谱方法优选衍生基团与完整肽离子和多个片段一起作为被动质量标签。本工作研究了五种线性ω-二甲基氨基酸（从2-（二甲氨基）-乙酸到6-（二甲氨基）-己酸）对胺基衍生化肽的碰撞断裂。衍生化胰蛋白酶肽的串联质谱显示不同的优先分解途径。与能量分辨质谱法一起，发现关闭末端二甲基氨基在衍生肽片段化中的积极参与是可能的。然而，在末端二甲基氨基和肽衍生化后形成的酰胺之间需要分离五个亚甲基。首次报道了用系统增加烷基链长度的线性ω-二甲基氨基酸衍生的肽的气相裂解。
Direct reductive methylation of peptides is a common method for quantitative proteomics. It is an active derivatization technique; with participation of the dimethylamino group, the derivatized peptides preferentially release intense a1 ions. The advantageous generation of a1 ions for quantitative proteomic profiling, however, is not desirable for targeted proteomic quantitation using multiple reaction monitoring mass spectrometry; this mass spectrometric method prefers the derivatizing group to stay with the intact peptide ions and multiple fragments as passive mass tags. This work investigated collisional fragmentation of peptides whose amine groups were derivatized with five linear ω-dimethylamino acids, from 2-(dimethylamino)-acetic acid to 6-(dimethylamino)-hexanoic acid. Tandem mass spectra of the derivatized tryptic peptides revealed different preferential breakdown pathways. Together with energy resolved mass spectrometry, it was found that shutting down the active participation of the terminal dimethylamino group in fragmentation of derivatized peptides is possible. However, it took a separation of five methylene groups between the terminal dimethylamino group and the amide formed upon peptide derivatization. For the first time, the gas-phase fragmentation of peptides derivatized with linear ω-dimethylamino acids of systematically increasing alkyl chain lengths is reported.
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影响因子：
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作者：
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