Development of a High Coverage Pseudotargeted Lipidomics Method Based on Ultra-High Performance Liquid Chromatography-Mass Spectrometry.
Development of a High Coverage Pseudotargeted Lipidomics Method Based on Ultra-High Performance Liquid Chromatography-Mass Spectrometry.
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基于超高效液相色谱-质谱联用技术的高覆盖度伪靶向脂质组学方法的开发
DOI：
10.1021/acs.analchem.8b01331
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发表时间：
2018-06-19
影响因子：
7.4
通讯作者：
Xu G
中科院分区：
文献类型：
--
作者：
Xuan Q;Hu C;Yu D;Wang L;Zhou Y;Zhao X;Li Q;Hou X;Xu G
脂质覆盖率在全面的脂质组学研究中至关重要，这些研究受到脂质结构高度多样性和脂质水平宽动态范围的挑战。目前最先进的脂质组学技术主要基于质谱（MS），包括直接注入MS，色谱-MS和基质辅助激光解吸电离（MALDI）成像MS，每种都有其优点和缺点。由于需要或可测量异构体和同量异位素，色谱-MS是首选的脂质分析。基于超高效液相色谱-高分辨质谱（UHPLC-HRMS）的非靶向脂质组学方法和基于超高效液相色谱-串联质谱（UHPLC-MS/MS）的靶向方法是色谱-质谱的两个代表性方法平台。脂质的高覆盖率是通过整合源自多个基质（例如，血浆、细胞和组织）和基于已知脂质的结构和色谱保留行为推测的预测脂质。共定义了3377个靶向脂质离子对，具有超过7000个脂质分子结构。假靶向脂质组学方法得到了很好的验证，在脂质组学分析的线性、精密度、重现性和回收率方面具有令人满意的分析特性。重要的是，它显示出比非靶向脂质组学方法更好的重复性和更高的脂质覆盖率。所开发的假靶向脂质组学方法的适用性被证明在定义与糖尿病相关的差异脂质。我们相信，全面的脂质组学研究将受益于已开发的高覆盖率假靶向脂质组学方法。
Lipid coverage is crucial in comprehensive lipidomics studies challenged by high diversity in lipid structures and wide dynamic range in lipid levels. Current state-of-the-art lipidomics technologies are mostly based on mass spectrometry (MS), including direct-infusion MS, chromatography-MS, and matrix-assisted laser desorption ionization (MALDI) imaging MS, each with its pros and cons. Due to the need or favorability for measurement of isomers and isobars, chromatography-MS is preferable for lipid profiling. The ultra-high performance liquid chromatography-high resolution mass spectrometry (UHPLC-HRMS)-based nontargeted lipidomics approach and UHPLC-tandem MS (UHPLC-MS/MS)-based targeted approach are two representative methodological platforms for chromatography-MS. In the present study, we developed a high coverage pseudotargeted lipidomics method combining the advantages of nontargeted and targeted lipidomics approaches. The high coverage of lipids was achieved by integration of the detected lipids derived from nontargeted UHPLC-HRMS lipidomics analysis of multiple matrices (e.g., plasma, cell, and tissue) and the predicted lipids speculated on the basis of the structure and chromatographic retention behavior of the known lipids. A total of 3377 targeted lipid ion pairs with over 7000 lipid molecular structures were defined. The pseudotargeted lipidomics method was well validated with satisfactory analytical characteristics in terms of linearity, precision, reproducibility, and recovery for lipidomics profiling. Importantly, it showed better repeatability and higher coverage of lipids than the nontargeted lipidomics method. The applicability of the developed pseudotargeted lipidomics method was testified in defining differential lipids related to diabetes. We believe that comprehensive lipidomics studies will benefit from the developed high coverage pseudotargeted lipidomics approach.
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