Xia Hanxue, Attygalle Athula B
Center for Mass Spectrometry, Department of Biomedical Engineering, Chemistry, and Biological Sciences, Stevens Institute of Technology, Hoboken, NJ, 07030, USA.
J Am Soc Mass Spectrom. 2017 Dec;28(12):2580-2587. doi: 10.1007/s13361-017-1806-9. Epub 2017 Sep 21.
The role of water vapor in transforming the thermodynamically preferred species of protonated benzocaine to the less favored protomer was investigated using helium-plasma ionization (HePI) in conjunction with ion-mobility mass spectrometry (IM-MS). The IM arrival-time distribution (ATD) recorded from a neat benzocaine sample desorbed to the gas phase by a stream of dry nitrogen and ionized by HePI showed essentially one peak for the O-protonated species. However, when water vapor was introduced to the enclosed ion source, within a span of about 150 ms the ATD profile changed completely to one dominated by the N-protonated species. Under spray-based ionization conditions, the nature and composition of the solvents have been postulated to play a decisive role in defining the manifested protomer ratios. In reality, the solvent vapors present in the ion source (particularly the ambient humidity) indirectly dictate the gas-phase ratio of the protomers. Evidently, the gas-phase protomer ratio established at the confinement of the ions is readjusted by the ion-activation that takes place during the transmission of ions to the vacuum. Although it has been repeatedly stated that ions can retain a "memory" of their solution structures because they can be kinetically trapped, and thereby represent their solution-based stabilities, we show that the initial airborne ions can undergo significant transformations in the transit through the intermediate vacuum zones between the ion source and the mass detector. In this context, we demonstrate that the kinetically trapped N-protomer of benzocaine can be untrapped by reducing the humidity of the enclosed ion source. Graphical Abstract ᅟ.
利用氦等离子体电离(HePI)结合离子淌度质谱(IM-MS),研究了水蒸气在将质子化苯佐卡因的热力学优势物种转化为较不利的异构体过程中的作用。从通过干燥氮气流解吸到气相并经HePI电离的纯苯佐卡因样品记录的IM到达时间分布(ATD)显示,O-质子化物种基本上只有一个峰。然而,当将水蒸气引入封闭的离子源时,在约150毫秒的时间跨度内,ATD谱完全改变为以N-质子化物种为主导的谱。在基于喷雾的电离条件下,已假定溶剂的性质和组成在确定表现出的异构体比例方面起决定性作用。实际上,离子源中存在的溶剂蒸气(特别是环境湿度)间接决定了异构体的气相比例。显然,在离子限制处建立的气相异构体比例会因离子传输到真空过程中发生的离子活化而重新调整。尽管人们反复指出离子可以保留其溶液结构的“记忆”,因为它们可以被动力学捕获,从而代表其基于溶液的稳定性,但我们表明,初始的空气传播离子在通过离子源和质量检测器之间的中间真空区域时会发生显著变化。在这种情况下,我们证明通过降低封闭离子源的湿度,可以使动力学捕获的苯佐卡因N-异构体解捕获。图形摘要ᅟ。