Metabolic profiling of Escherichia coli by ion mobility-mass spectrometry with MALDI ion source.

Metabolic profiling of Escherichia coli by ion mobility-mass spectrometry with MALDI ion source.
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DOI:
10.1002/jms.1850
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发表时间:
2010-12
影响因子:
2.3
通讯作者:
Hill, Herbert H., Jr.
Hill, Herbert H., Jr.
中科院分区:
化学4区
文献类型:
--
作者:
Dwivedi, Prabha;Puzon, Geoffery;Tam, Maggie;Langlais, Denis;Jackson, Shelley;Kaplan, Kimberly;Siems, William F.;Schultz, Albert J.;Xun, Luying;Woodsd, Amina;Hill, Herbert H., Jr.

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利用质谱仪进行全面的代谢组分析往往会导致复杂的质谱图和难以分析的数据,因为代谢组中含有大量的小分子信号。此外,单靠质谱学很难测量同分异构体和手性、构象和结构异构体。当增加基质辅助激光解吸电离源(MALDI)时,进一步增加了难度和复杂性。MALDI在低质量区域(<1500 Da)产生的分析物信号和基质离子信号之间的信号干扰导致仅通过质谱学难以检测和/或鉴定代谢物。然而,离子迁移率光谱(IMS)与质谱仪(IM-MS)联用为测量化学品中细微的结构差异提供了一种快速分析工具。IMS根据气相离子的大小与电荷比来分离它们。本研究首次报道了MALDI在离子迁移率-飞行时间质谱仪(IM-TOFMS)测量生物基质小分子中的应用,并证明了离子信号二维色散的优越性。报道了用MALDI-TOFMS、MALDI-IM-TOFMS和ESI-IM-TOFMS(电喷雾电离)对大肠杆菌代谢组进行定性比较。结果表明,在质量分析之前的迁移率分离通过在测量中增加维度来增加峰容量。迁移率分离还可以通过在迁移率空间中分离基质信号和非基质信号来检测以基质离子为主的低质量范围(m/z<1500 Da)的代谢物。
Comprehensive metabolome analysis using mass spectrometry (MS) often results in a complex mass spectrum and difficult data analysis resulting from the signals of numerous small molecules in the metabolome. In addition, mass spectrometry alone has difficulty measuring isobars and chiral, conformational, and structural isomers. When a matrix assisted laser desorption ionization source (MALDI) is added, the difficulty and complexity are further increased. Signal interference between analyte signals and matrix ion signals produced by MALDI in the low mass region (<1500 Da) cause detection and or identification of metabolites difficult by mass spectrometry alone. However, ion mobility spectrometry (IMS) coupled with MS (IM-MS) provides a rapid analytical tool for measuring subtle structural differences in chemicals. IMS separates gas phase ions based on their size-to-charge ratio. This study, for the first time, reports the application of MALDI to the measurement of small molecules in a biological matrix by Ion Mobility-Time of Flight Mass Spectrometry (IM-TOFMS) and demonstrates the advantage of ion-signal dispersion in the second dimension. Qualitative comparisons between metabolic profiling of the Escherichia coli metabolome by MALDI-TOFMS, MALDI-IM-TOFMS, and ESI-IM-TOFMS (electrospray ionization) are reported. Results demonstrate that mobility separation prior to mass analysis increases peak-capacity through added dimensionality in measurement. Mobility separation also allows detection of metabolites in the matrix-ion dominated low-mass range (m/z < 1500 Da) by separating matrix-signals from non-matrix signals in mobility space.
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