Triboelectric Nanogenerator Ion Mobility-Mass Spectrometry for In-Depth Lipid Annotation.
Triboelectric Nanogenerator Ion Mobility-Mass Spectrometry for In-Depth Lipid Annotation.
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DOI：
10.1021/acs.analchem.0c05145
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发表时间：
2021-04-06
影响因子：
7.4
通讯作者：
Fernández FM
中科院分区：
文献类型：
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作者：
Bouza M;Li Y;Wang AC;Wang ZL;Fernández FM
脂质在细胞膜完整性、信号传递和能量储存中起着关键作用。然而，深入的脂类结构表征仍然是具有挑战性的，在脂类组学实验中通常不可能实现。碰撞诱导解离(CID)串联质谱仪(MS/MS)、离子迁移率(IM)光谱和超高效液相色谱(UHLC)等技术还不能高通量地完全表征脂类的双键和sn链位置。在这里，我们报告了使用大面积摩擦电纳米发电机(TENG)结合时间定向平行(TAP)碎裂IM-MS分析来表征脂类的结构特征的能力。Teng电离过程中的气相脂质环氧化，通过TAP IM-MS与迁移率分辨的MS3相耦合，使得能够获得关于脂质C═C双键的存在和位置、脂肪酰基sn链的位置和组成以及顺/反几何C═C异构体的详细信息。所提出的方法被证明是有用的鸟枪式类脂组学分析生物样品的脂类提取物，使详细的注释大量的类脂异构体。
Lipids play a critical role in cell membrane integrity, signaling, and energy storage. However, in-depth structural characterization of lipids is still challenging and not routinely possible in lipidomics experiments. Techniques such as collision-induced dissociation (CID) tandem mass spectrometry (MS/MS), ion mobility (IM) spectrometry, and ultrahigh-performance liquid chromatography are not yet capable of fully characterizing double-bond and sn-chain position of lipids in a high-throughput manner. Herein, we report on the ability to structurally characterize lipids using large-area triboelectric nanogenerators (TENG) coupled with time-aligned parallel (TAP) fragmentation IM-MS analysis. Gas-phase lipid epoxidation during TENG ionization, coupled to mobility-resolved MS3 via TAP IM-MS, enabled the acquisition of detailed information on the presence and position of lipid C═C double bonds, the fatty acyl sn-chain position and composition, and the cis/trans geometrical C═C isomerism. The proposed methodology proved useful for the shotgun lipidomics analysis of lipid extracts from biological samples, enabling the detailed annotation of numerous lipid isobars.