Relative Quantitation of Unsaturated Phosphatidylcholines Using 193 nm Ultraviolet Photodissociation Parallel Reaction Monitoring Mass Spectrometry,Journal of the American Chemical Society

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Relative Quantitation of Unsaturated Phosphatidylcholines Using 193 nm Ultraviolet Photodissociation Parallel Reaction Monitoring Mass Spectrometry
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-09-06 , DOI: 10.1021/jacs.1c05295
Luis A Macias ₁ , Kyana Y Garza ₁ , Clara L Feider ₁ , Livia S Eberlin ₁ , Jennifer S Brodbelt ₁

Affiliation

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.

中文翻译：

使用 193 nm 紫外光解离平行反应监测质谱法对不饱和磷脂酰胆碱进行相对定量

超越脂肪酸水平的甘油磷脂的结构表征已成为脂质组学的主要努力，为增进对脂质代谢与疾病状态之间复杂关系的理解提供了机会。然而，区分微妙的脂质结构特征仍然是实施传统串联质谱 (MS/MS) 技术的高通量工作流程的主要挑战，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联用，利用紫外光解离 (UVPD) 质谱的双键定位能力，产生双键异构体特异性响应，用于相对定量。该策略提供了生物提取物中磷脂酰胆碱磷脂双键水平的脂质组学表征。除了定量单不饱和脂质外，还可以定量掺入异构多不饱和脂肪酸的磷脂。使用该技术，比较人类正常和肿瘤乳腺组织中的磷脂酰胆碱异构体比率，以揭示与疾病状态相关的显着结构变化。

更新日期：2021-09-15

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