A new strategy for MS/MS data acquisition applying multiple data dependent experiments on Orbitrap mass spectrometers in non-targeted metabolomic applications
A new strategy for MS/MS data acquisition applying multiple data dependent experiments on Orbitrap mass spectrometers in non-targeted metabolomic applications
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DOI：
10.1007/s11306-014-0763-6
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发表时间：
2015-10-01
期刊：
影响因子：
3.6
通讯作者：
Dunn, Warwick B.
中科院分区：
文献类型：
--
作者：
Mullard, Graham;Allwood, James W.;Dunn, Warwick B.
代谢物的标注和鉴定是目前非靶向代谢组学研究的瓶颈。虽然精确测量m/z在UPLC-MS应用中被常规应用于代谢物的推定注释，但需要获取MS/MS或MS (n)数据来推断结构信息，进一步减少化学搜索空间，并通过与质谱数据库相比，为代谢物注释提供更大的信心。在此，我们提出了一种创新的数据依赖采集（DDA）新策略，用于在线MS/MS数据采集，同时在LTQ-Orbitrap质谱上进行全扫描代谢物分析。我们建议应用不同的和集成的DDA MS/MS实验，以增加获得MS/MS数据的独特代谢物的覆盖率。我们首次证明了CID和高能碰撞解离离子激活方法的综合应用，多种不同的活化能和窄的前体离子m/z范围（100或300）用于获取MS/MS光谱提供了补充信息，并增加了获取MS/MS数据的独特代谢物的数量。本文的策略提供了一种不同的数据获取方法，以增加非靶向代谢组学研究中代谢物注释目的获得的独特MS/MS质谱的数量。MS/MS数据可根据通讯作者的要求提供。
The annotation and identification of metabolites is a current bottleneck in non-targeted metabolomics studies. Although accurate measurement of m/z is applied routinely in UPLC-MS applications to putatively annotate metabolites, the acquisition of MS/MS or MS (n) data is required to deduce structural information, further reducing the chemical search-space and providing greater confidence in metabolite annotation by comparison to mass spectral databases. Here we propose an innovative new strategy for data dependent acquisition (DDA) for on-line MS/MS data acquisition in parallel to full-scan metabolite profiling on LTQ-Orbitrap mass spectrometers. We recommend the application of different and integrated DDA MS/MS experiments to increase the coverage of unique metabolites for which MS/MS data were acquired. We demonstrate, for the first time, that the integrated application of both CID and higher-energy collisional dissociation ion activation methods, multiple different activation energies and narrow precursor ion m/z ranges of 100 or 300 for acquisition of MS/MS spectra provide complementary information and increases the number of unique metabolites for which MS/MS data is acquired. The strategies herein provide a different approach for data acquisition to increase the number of unique MS/MS mass spectra acquired for metabolite annotation purposes in non-targeted metabolomics studies. MS/MS data are available on request from the corresponding author.