Mass Spectrometry Data Repository Enhances Novel Metabolite Discoveries with Advances in Computational Metabolomics
Mass Spectrometry Data Repository Enhances Novel Metabolite Discoveries with Advances in Computational Metabolomics
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DOI：
10.3390/metabo9060119
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发表时间：
2019-06
期刊：
影响因子：
4.1
通讯作者：
H. Tsugawa;Aya Satoh;Haruki Uchino;T. Cajka;Makoto Arita;Masanori Arita
中科院分区：
文献类型：
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作者：
H. Tsugawa;Aya Satoh;Haruki Uchino;T. Cajka;Makoto Arita;Masanori Arita
质谱原始数据库，包括Metabolomics和MetaboLights，有助于提高代谢组学研究的透明度，并通过使用更新的计算代谢组学工具进行重新分析，发现生物学方面的新见解。在此，我们重新分析了先前发表的来自9种藻类的脂质组学数据，导致1437种脂质的注释与先前的结果相比增加了40%。具体地说，二酰基甘油-羧基羟基-甲基胆碱（DGCC）在Pavlova lutheri和侧鞭金藻carterae中，葡萄糖醛酸二酰基甘油（GlcADG）在Euglena gracilis中，和P. carterae中，磷脂酰甲醇（PMeOH）在E.利用丰富的脂质光谱数据库对小球藻中的氧化磷脂（氧化磷脂酰胆碱，OxPC;磷脂酰乙醇胺，OxPE;磷脂酰甘油，OxPG;磷脂酰肌醇，OxPI）进行了新的表征。此外，我们整合了来自数据独立串联质谱（DIA-MS/MS）采集的非靶向和靶向分析的数据，特别是所有理论碎片离子MS/MS（SWATH-MS/MS）光谱的连续窗口采集，以增加脂质组学注释覆盖率。通过MS-DIAL非靶向分析创建脂质前体和诊断离子的全局库后，通过追踪酰基链组成中涉及的特定产物离子，在MRMPROBS靶向分析中解析共洗脱的DIA-MS/MS光谱。我们的研究结果表明，代谢物定量的基础上DIA-MS/MS色谱图是有点不如MS 1为中心的定量，而注释覆盖率优于那些非靶向分析的数据依赖和DIA-MS/MS数据。因此，非靶向和靶向方法的综合分析是必要的，以提取最大量的代谢组信息，我们的研究结果展示了数据存储库的价值，用于发现脂质生物学的新见解。
Mass spectrometry raw data repositories, including Metabolomics Workbench and MetaboLights, have contributed to increased transparency in metabolomics studies and the discovery of novel insights in biology by reanalysis with updated computational metabolomics tools. Herein, we reanalyzed the previously published lipidomics data from nine algal species, resulting in the annotation of 1437 lipids achieving a 40% increase in annotation compared to the previous results. Specifically, diacylglyceryl-carboxyhydroxy-methylcholine (DGCC) in Pavlova lutheri and Pleurochrysis carterae, glucuronosyldiacylglycerol (GlcADG) in Euglena gracilis, and P. carterae, phosphatidylmethanol (PMeOH) in E. gracilis, and several oxidized phospholipids (oxidized phosphatidylcholine, OxPC; phosphatidylethanolamine, OxPE; phosphatidylglycerol, OxPG; phosphatidylinositol, OxPI) in Chlorella variabilis were newly characterized with the enriched lipid spectral databases. Moreover, we integrated the data from untargeted and targeted analyses from data independent tandem mass spectrometry (DIA-MS/MS) acquisition, specifically the sequential window acquisition of all theoretical fragment-ion MS/MS (SWATH-MS/MS) spectra, to increase the lipidomic annotation coverage. After the creation of a global library of precursor and diagnostic ions of lipids by the MS-DIAL untargeted analysis, the co-eluted DIA-MS/MS spectra were resolved in MRMPROBS targeted analysis by tracing the specific product ions involved in acyl chain compositions. Our results indicated that the metabolite quantifications based on DIA-MS/MS chromatograms were somewhat inferior to the MS1-centric quantifications, while the annotation coverage outperformed those of the untargeted analysis of the data dependent and DIA-MS/MS data. Consequently, integrated analyses of untargeted and targeted approaches are necessary to extract the maximum amount of metabolome information, and our results showcase the value of data repositories for the discovery of novel insights in lipid biology.