Park Nathaneal A, Glish Gary L, Dick Jeffrey E
Department of Chemistry, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina27599, United States.
Lineberger Comprehensive Cancer Center, School of Medicine, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina27599, United States.
J Am Soc Mass Spectrom. 2023 Feb 1;34(2):320-327. doi: 10.1021/jasms.2c00338. Epub 2023 Jan 11.
Electrospray ionization (ESI) is a powerful ionization technique that can generate charged solvent droplets and bare analyte ions from sample solutions. Despite seeing extensive use in mass spectrometry due in part to the low internal energy deposited into the ions formed during ionization, some unknowns persist regarding the exact dynamics of droplet breakup and molecule behavior during spray, and research is still underway regarding how various types of molecules acquire charge during the ESI process. Previously, the authors introduced a novel aerosol measurement technique, particle-into-liquid sampling for nanoliter electrochemical reactions (PILSNER). The current work introduces a new method utilizing PILSNER for the examination of the particles generated during ESI using simple analysis techniques with a commercially available potentiostat. This technique is applied in this work for the detection of charges on electrosprayed droplets, including the estimation of the number of charges on individual ESI droplets using a fluorescent proxy. This technique provides an additional tool for the exploration of the complex process of droplet generation and ion liberation during ESI.
电喷雾电离（ESI）是一种强大的电离技术，它可以从样品溶液中产生带电溶剂液滴和裸分析物离子。尽管由于在电离过程中形成的离子所沉积的内能较低，ESI在质谱分析中得到了广泛应用，但关于喷雾过程中液滴破裂的确切动力学和分子行为仍存在一些未知因素，并且关于各种类型的分子在ESI过程中如何获得电荷的研究仍在进行中。此前，作者介绍了一种新颖的气溶胶测量技术，即用于纳升电化学反应的液滴进样（PILSNER）。目前的工作引入了一种利用PILSNER的新方法，通过使用市售恒电位仪的简单分析技术来检测ESI过程中产生的颗粒。这项技术在本工作中用于检测电喷雾液滴上的电荷，包括使用荧光替代物估计单个ESI液滴上的电荷量。该技术为探索ESI过程中液滴生成和离子释放的复杂过程提供了一个额外的工具。
