Relative Quantitation of Unsaturated Phosphatidylcholines Using 193 nm Ultraviolet Photodissociation Parallel Reaction Monitoring Mass Spectrometry.
Relative Quantitation of Unsaturated Phosphatidylcholines Using 193 nm Ultraviolet Photodissociation Parallel Reaction Monitoring Mass Spectrometry.
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DOI：
10.1021/jacs.1c05295
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发表时间：
2021-09-15
影响因子：
15
通讯作者：
Brodbelt JS
中科院分区：
文献类型：
--
作者：
Macias LA;Garza KY;Feider CL;Eberlin LS;Brodbelt JS
超过脂肪酸水平的甘油磷脂的结构表征已经成为脂类组学中的一项主要工作，这为进一步了解脂代谢和疾病状态之间的复杂关系提供了机会。然而，区分细微的脂类结构特征仍然是实现传统串联质谱仪(MS/MS)技术的高通量工作流的主要挑战，阻碍了定量策略的分子深度。在这里，反相液相色谱与平行反应质谱仪相结合，利用紫外光解离(UVPD)质谱学的双键定位能力，产生双键异构体的特定响应，用于相对定量。该策略提供了从生物提取物中提取的磷脂酰胆碱磷脂在双键水平上的脂组特征。除了定量单不饱和脂肪外，还实现了含有异构体多不饱和脂肪酸的磷脂的定量。利用这项技术，比较了人类正常和肿瘤乳腺组织中磷脂酰胆碱异构体的比率，以揭示与疾病状态相关的显著结构变化。
Structural characterization of glycerophospholipids beyond the fatty acid level has become a major endeavor in lipidomics, presenting an opportunity to advance the understanding of the intricate relationship between lipid metabolism and disease state. Distinguishing subtle lipid structural features, however, remains a major challenge for high-throughput workflows that implement traditional tandem mass spectrometry (MS/MS) techniques, stunting the molecular depth of quantitative strategies. Here, reversed phase liquid chromatography is coupled to parallel reaction mass spectrometry utilizing the double bond localization capabilities of ultraviolet photodissociation (UVPD) mass spectrometry to produce double bond isomer specific responses that are leveraged for relative quantitation. The strategy provides lipidomic characterization at the double bond level for phosphatidylcholine phospholipids from biological extracts. In addition to quantifying monounsaturated lipids, quantitation of phospholipids incorporating isomeric polyunsaturated fatty acids is also achieved. Using this technique, phosphatidylcholine isomer ratios are compared across human normal and tumor breast tissue to reveal significant structural alterations related to disease state.
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影响因子：
7.4
作者：
Klein DR;Holden DD;Brodbelt JS
通讯作者：
Brodbelt JS
通过质谱法对组织中脂质生物化学的MALDI成像。
影响因子：
62.1
作者：
Berry, Karin A. Zemski;Hankin, Joseph A.;Barkley, Robert M.;Spraggins, Jeffrey M.;Caprioli, Richard M.;Murphy, Robert C.
通讯作者：
Murphy, Robert C.
影响因子：
4.3
作者：
Hsu FF
通讯作者：
Hsu FF
影响因子：
16.1
作者：
Butler LM;Perone Y;Dehairs J;Lupien LE;de Laat V;Talebi A;Loda M;Kinlaw WB;Swinnen JV
通讯作者：
Swinnen JV
影响因子：
7.4
作者：
Klein DR;Brodbelt JS
通讯作者：
Brodbelt JS