分析化学2025，Vol.53Issue(5)：740-748,9.DOI:10.19756/j.issn.0253-3820.251043
基于串级离子迁移谱的离子筛选及反应性研究
Ion Filtering and Reactivity Investigation Based on Tandem Ion Mobility Spectrometry
摘要
Abstract
In analytical techniques such as ion mobility spectrometry(IMS)and mass spectrometry(MS),the ionization efficiency of target analytes is primarily constrained by the type of ionization source and factors such as the species and number density of the reactant ions.Systematic investigation into the reactivity differences of various reactant ions under varying conditions can not only significantly enhance the detection sensitivity of target compound product ions but also provide a theoretical foundation for establishing efficient detection methods based on ion-molecule reaction mechanisms.In this study,the pressure of a pressure-tunable photoionization tandem ion mobility spectrometry(PI-tandem-IMS)was reduced from ambient pressure(100 kPa)to low pressure(20 kPa)to systematically examine the reactivity differences between two negative reactant ions,CO3-and CO4-,and methyl salicylate(MeSA)under varying pressures.When the pressure decreased,the increased relative signal intensity of CO4-significantly influenced the detection sensitivity of the characteristic product ion[MeSA·O2]-.Based on differences in ion mobility(k0),the delay time for the opening of TPG2 was adjusted to selectively inject CO-3 and CO-4 in the drift region 2.Independent characterization of the reactivity of these reactant ions with MeSA in the reaction region confirmed that CO4-exhibited superior reactivity toward MeSA.The theoretical model revealed an Arrhenius plot for the ion-molecule reaction between CO4-and MeSA,showing a positive correlation between the reaction rate coefficient(k)and temperature,the activation energy Ea was 62.45 kJ/mol.Furthermore,controlling parameters such as pressure or temperature significantly influenced the progression of this ion-molecule reaction,demonstrating the technical advantages of PI-tandem-IMS in mechanistic studies and regulation of ion-molecule reactions.关键词
离子迁移谱/光电离/离子筛选/离子反应性Key words
Ion mobility spectrometry/Photoionization/Ion filtering/Ion reactivity引用本文复制引用
徐一仟,杨其穆,潘慢慢,蒋丹丹,陈创,李海洋..基于串级离子迁移谱的离子筛选及反应性研究[J].分析化学,2025,53(5):740-748,9.基金项目
国家自然科学基金项目(Nos.22027804,21974141)、大连市科技人才创新支持计划项目(No.2024RY022)和中国科学院大连化学物理研究所创新研究基金项目(Nos.DICP I202422,DICP I202442)资助. Supported by the National Natural Science Foundation of China(Nos.22027804,21974141),the Dalian High-Level Talent Innovation Support Project(No.2024RY022),and the Dalian Institute of Chemical Physics(Nos.DICP I202422,DICP I202442). （Nos.22027804,21974141）
