Nonuniform Sampling Acquisition of Two-Dimensional Fourier Transform Ion Cyclotron Resonance Mass Spectrometry for Increased Mass Resolution of Tandem Mass Spectrometry Precursor Ions
Nonuniform Sampling Acquisition of Two-Dimensional Fourier Transform Ion Cyclotron Resonance Mass Spectrometry for Increased Mass Resolution of Tandem Mass Spectrometry Precursor Ions
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DOI：
10.1021/acs.analchem.7b01850
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发表时间：
2017-09-05
影响因子：
7.4
通讯作者：
Rolando, Christian
中科院分区：
文献类型：
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作者：
Bray, Fabrice;Bouclon, Julien;Rolando, Christian
获得完整的MS/MS图谱的碎片和前体的复杂混合物-没有联用色谱分离的数据独立的采集是一个挑战，在质谱，这是解决了二维（2D）傅里叶变换离子回旋共振质谱（FTICR MS）。到目前为止，2D FTICR MS只提供了一个中等分辨率的前体离子，因为这种分辨率是有限的演变间隔步骤的数量，扫描的数量，采集时间和样品消耗成正比。已经需要过夜采集来达到类似四极质量过滤器的单位质量分辨率。在这里，我们报告说，2D FTICR MS使用非均匀采样（NUS）通过随机跳过点在第一维对应的前体选择获得访问，数据处理后，包含在一个复杂的混合物中的相同的结构信息。分辨率大致随着NUS比率的倒数增加，在NUS 1/32处高达26倍，导致与相同分辨率下的经典采集相比，采集时间以相同比率减少。作为一个例子，天然油的分析。
Obtaining the full MS/MS map for fragments and precursors of complex mixtures-without hyphenation with chromatographic separation by a data-independent acquisition is a challenge in mass spectrometry which is solved by two-dimensional (2D) Fourier transform ion cyclotron resonance mass spectrometry (FTICR MS). Until now 2D FTICR MS afforded only a moderate resolution for precursor ion since this resolution is limited by the number of evolution interval steps to which the number of scans, the acquisition time, and the sample consumption are proportional. An overnight acquisition is already required to reach a quadrupole mass filter-like unit mass resolution. Here, we report that 2D FTICR MS using nonuniform sampling (NUS) obtained by randomly skipping points in the first dimension corresponding to the precursor selection gives access, after data processing, to the same structural information contained in a complex mixture. The resolution increases roughly as the inverse of the NUS ratio, up to 26 times at NUS 1/32, leading to an acquisition time reduced in the same ratio compared to a classical acquisition at the same resolution. As an example, the analysis of a natural oil is presented.