Novel ionization processes for use in mass spectrometry: 'Squeezing' nonvolatile analyte ions from crystals and droplets
Novel ionization processes for use in mass spectrometry: 'Squeezing' nonvolatile analyte ions from crystals and droplets
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DOI：
10.1002/rcm.8269
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发表时间：
2019-07-01
影响因子：
2
通讯作者：
Trimpin, Sarah
中科院分区：
文献类型：
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作者：
Trimpin, Sarah
有幸与我的团队和合作者一起，在发现新的电离过程中发挥了关键作用，我们将这些新的电离过程开发成灵活、灵敏、快速、可靠和强大的新电离技术和方法，用于质谱学(MS)。我们目前的研究重点是如何最好地了解、改进和使用这些新的电离过程，这些电离过程将挥发性和非挥发性化合物从固体或液体转化为气相离子，供MS分析，例如使用质量选择碎裂和离子迁移率光谱，以提供可重复性、准确性和改进的质量和漂移时间分辨率。在我看来，顶峰是2012年在中压基质辅助激光解吸/电离(MALDI)源上发现的真空基质辅助电离(VMAI)，无需使用激光、高电压或任何其他附加能量。只需将基质：分析物暴露在质谱仪的亚大气压下，即可启动电离。这些发现最初被三种不同的科学期刊拒绝，评论内容分别是“这是如何起作用的？”、“收费从何而来？”以及“它在分析上没有用处”。与此同时，我们和其他人在对机制没有完全了解的情况下，展示了分析的实用性。在现实中，MALDI和电喷雾电离在科学上得到了广泛的应用，尽管经过了30年的使用和优化，它们的作用机理仍然存在争议。这一观点涵盖了在MS中使用的新型电离过程的应用和机制方面，这些过程指导我们开发仪器，并提供了我们关于它们如何与传统电离过程相关的观点。
Together with my group and collaborators, I have been fortunate to have had a key role in the discovery of new ionization processes that we developed into new flexible, sensitive, rapid, reliable, and robust ionization technologies and methods for use in mass spectrometry (MS). Our current research is focused on how best to understand, improve, and use these novel ionization processes which convert volatile and nonvolatile compounds from solids or liquids into gas-phase ions for analysis by MS using e.g. mass-selected fragmentation and ion mobility spectrometry to provide reproducible, accurate, and improved mass and drift time resolution. In my view, the apex was the discovery of vacuum matrix-assisted ionization (vMAI) in 2012 on an intermediate pressure matrix-assisted laser desorption/ionization (MALDI) source without the use of a laser, high voltages, or any other added energy. Only exposure of the matrix:analyte to the sub-atmospheric pressure of the mass spectrometer was necessary to initiate ionization. These findings were initially rejected by three different scientific journals, with comments related to 'how can this work?', 'where do the charges come from?', and 'it is not analytically useful'. Meanwhile, we and others have demonstrated analytical utility without a complete understanding of the mechanism. In reality, MALDI and electrospray ionization are widely used in science and their mechanisms are still controversially discussed despite use and optimization of now 30 years. This Perspective covers the applications and mechanistic aspects of the novel ionization processes for use in MS that guided us in instrument developments, and provides our perspective on how they relate to traditional ionization processes.