Voltage-Controlled Divergent Cascade of Electrochemical Reactions for Characterization of Lipids at Multiple Isomer Levels Using Mass Spectrometry.
Voltage-Controlled Divergent Cascade of Electrochemical Reactions for Characterization of Lipids at Multiple Isomer Levels Using Mass Spectrometry.
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DOI：
10.1021/acs.analchem.2c02375
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发表时间：
2022-09-20
影响因子：
7.4
通讯作者：
Wang, Fen
中科院分区：
文献类型：
--
作者：
Tang, Shuli;Yan, Xin;Ke, Yuepeng;Chen, Xi;Wang, Fen
在单一系统中级联发散反应是非常可取的，因为它们的内在效率和潜力，以实现复杂的生物分子的多级结构表征。在这项工作中，两个电化学反应，界面电环氧化和钴阳极腐蚀，发散级联在纳米电喷雾（nESI），并可以在不同的电压切换。我们将这些反应应用于使用质谱（MS）在多个异构体水平上的脂质鉴定，这在结构脂质组学中仍然是一个巨大的挑战。不同的级联反应在不同电压下原位衍生脂质以产生环氧化脂质和钴加合物脂质。然后，这些脂质在低能量碰撞诱导解离（CID）后片段化，产生诊断片段以指示不能通过天然脂质的低能量CID实现的C=C位置和sn位置。我们已经证明，脂质结构异构体显示出显着不同的配置文件中的健康和癌小鼠前列腺样本的分析使用这种策略。发散级联反应在脂质鉴定中的应用允许简单地通过在单个实验中调整nESI电压来对脂质头基、脂肪酰基链、C=C位置和sn位置进行四合一分析。这一特点以及它的低样品消耗，不需要额外的设备，和定量分析能力显示了它在脂质组学中的巨大潜力。
Cascading divergent reactions in a single system is highly desirable for their intrinsic efficiency and potential to achieve multilevel structural characterization of complex biomolecules. In this work, two electrochemical reactions, interfacial electro-epoxidation and cobalt anodic corrosion, are divergently cascaded in nanoelectrospray (nESI) and can be switched at different voltages. We applied these reactions to lipid identification at multiple isomer levels using mass spectrometry (MS), which remains a great challenge in structural lipidomics. The divergent cascade reactions in situ derivatize lipids to produce epoxidized lipids and cobalt-adducted lipids at different voltages. These lipids are then fragmented upon low-energy collision-induced dissociation (CID), generating diagnostic fragments to indicate C=C locations and sn-positions that cannot be achieved by the low-energy CID of native lipids. We have demonstrated that lipid structural isomers show significantly different profiles in the analysis of healthy and cancerous mouse prostate samples using this strategy. The application of divergent cascade reactions in lipid identification allows the four-in-one analysis of lipid headgroups, fatty acyl chains, C=C locations, and sn-positions simply by tuning the nESI voltages within a single experiment. This feature as well as its low sample consumption, no need for an extra apparatus, and quantitative analysis capability show its great potential in lipidomics.
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影响因子：
16.6
作者：
Dutta, Soumen;Kumari, Nitee;Lee, In Su
通讯作者：
Lee, In Su
DOI：
10.1073/pnas.1700677114
发表时间：
2017-03-28
影响因子：
11.1
作者：
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作者：
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通讯作者：
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影响因子：
4.3
作者：
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通讯作者：
Mueller, Michael
影响因子：
7.4
作者：
Baba, Takashi;Campbell, J. Larry;Baker, Paul R. S.
通讯作者：
Baker, Paul R. S.