Broadband ion mobility deconvolution for rapid analysis of complex mixtures
Broadband ion mobility deconvolution for rapid analysis of complex mixtures
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用于快速分析复杂混合物的宽带离子淌度解卷积
DOI：
10.1039/c8an00193f
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发表时间：
2018
期刊：
影响因子：
--
通讯作者：
Solouki, Touradj
中科院分区：
文献类型：
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作者：
Pettit, Michael E.;Brantley, Matthew R.;Donnarumma, Fabrizio;Murray, Kermit K.;Solouki, Touradj
高分辨率离子迁移率（IM）允许在高通量IM质谱（IM-MS）实验中准确表征复杂混合物。我们先前证明，可以使用自动离子迁移率去卷积（AIMD）软件从IM未解析的IM/碰撞诱导解离（CID）后MS数据中提取纯组分IM-MS数据[Matthew Brantley，Behrooz Zekavat，Brett哈珀，Rachel Mason和Touradj Solouki，J. Am.质谱学会，2014，25，1810-1819]。在我们之前的报告中，我们利用四极杆离子过滤器在IM/CID MS后对IM未分离的单一同位素物质进行m/z分离。在这里，我们利用宽带IM-MS去卷积策略来消除成功去卷积IM未分离峰的m/z分离要求。宽带数据采集具有吞吐量和多路复用优势;因此，消除离子分离步骤减少了实验运行时间，从而将AIMD的适用性扩展到高吞吐量自下而上的蛋白质组学。我们证明了两个独立的和不相关的IM未分辨异构体对的宽带IM-MS去卷积（即，一对异构的六肽和一对异构的三肽）。此外，我们表明，宽带IM-MS反卷积提高了高通量自下而上的表征大鼠脑组织的蛋白水解消化。据我们所知，这份手稿是第一个报告成功的反卷积纯组分IM和MS数据从IM辅助数据独立分析（DIA）或HDMSE数据集。
High resolving power ion mobility (IM) allows for accurate characterization of complex mixtures in high-throughput IM mass spectrometry (IM-MS) experiments. We previously demonstrated that pure component IM-MS data can be extracted from IM unresolved post-IM/collision-induced dissociation (CID) MS data using automated ion mobility deconvolution (AIMD) software [Matthew Brantley, Behrooz Zekavat, Brett Harper, Rachel Mason, and Touradj Solouki, J. Am. Soc. Mass Spectrom., 2014, 25, 1810–1819]. In our previous reports, we utilized a quadrupole ion filter for m/z-isolation of IM unresolved monoisotopic species prior to post-IM/CID MS. Here, we utilize a broadband IM-MS deconvolution strategy to remove the m/z-isolation requirement for successful deconvolution of IM unresolved peaks. Broadband data collection has throughput and multiplexing advantages; hence, elimination of the ion isolation step reduces experimental run times and thus expands the applicability of AIMD to high-throughput bottom-up proteomics. We demonstrate broadband IM-MS deconvolution of two separate and unrelated pairs of IM unresolved isomers (viz., a pair of isomeric hexapeptides and a pair of isomeric trisaccharides) in a simulated complex mixture. Moreover, we show that broadband IM-MS deconvolution improves high-throughput bottom-up characterization of a proteolytic digest of rat brain tissue. To our knowledge, this manuscript is the first to report successful deconvolution of pure component IM and MS data from an IM-assisted data-independent analysis (DIA) or HDMSE dataset.