基于真空紫外灯的光电离质谱在催化反应过程监测中的应用  

Application of Vacuum Ultraviolet Lamp-based Photoionization Mass Spectrometry in the Monitoring of Catalytic Reaction Processes

作　　者：吴称心 花磊[1] 陈平[1] 蒋吉春 李金旭[1] 李海洋[1] WU Chen-xin;HUA Lei;CHEN Ping;JIANG Ji-chun;LI Jin-xu;LI Hai-yang(Liaoning Key Laboratory of Mass Spectrometry Technology and Instrumentation,Key Laboratory of Separation Science for Analytical Chemistry,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China)

机构地区：[1]中国科学院大连化学物理研究所,中国科学院分离分析化学重点实验室,辽宁省质谱技术与仪器重点实验室,辽宁大连116023

出　　处：《质谱学报》2024年第1期44-56,I0002,共14页Journal of Chinese Mass Spectrometry Society

基　　金：国家自然科学基金(22027804,22174142)。

摘　　要：催化反应机理研究是一个关键且极具挑战性的课题。在线监测催化反应过程中反应物、中间体和产物,可为复杂的催化反应网络、反应路径和反应动力学研究提供证据。真空紫外光电离质谱(VUV-PIMS)具有软电离、高灵敏度的优势,已成为备受关注的催化反应实时在线监测技术。本文综述了VUV-PIMS技术的发展情况,特别是基于真空紫外灯的光电离源研究进展,介绍了其在催化反应过程中稳定产物和活性中间体实时在线监测方面的最新应用,并针对催化反应过程精准表征的需求,对VUV-PIMS未来的发展趋势进行展望。The study of catalytic reaction mechanism is a critical and extremely challenging project.Online monitoring of reactants,intermediates and products during catalytic reactions can provide key evidence for the in-depth study of complex catalytic reaction networks,reaction pathways and reaction kinetics.As an online mass spectrometry based on soft ionization technique,vacuum ultraviolet photoionization mass spectrometry(VUV-PIMS)has proven itself as a versatile and powerful analytical technique for online and real-time process monitoring,which has gradually become a highly concerned characterization technique for catalytic reaction processes due to its advantages of high molecular ion yield,simple spectrum interpretation and high sensitivity.Compared with other commonly used synchrotron radiation and laser-based VUV light sources,the low pressure discharge lamps filled with various rare gases are compact,easy to operate,and low cost,such as krypton discharge lamps.However,the relatively low photon intensity of these lamps limits their applications.The efforts have been taken to develop stronger VUV light sources or lamp-based efficient combined ion sources to solve this issue.In this paper,the development of VUV-PIMS technology,especially the research progress of photoionization ion sources based on the VUV lamp,were reviewed,such as high-pressure photoionization(HPPI)source,single photon ionization-photoelectron ionization(SPI-PEI)combined ion source,and single photon ionization-chemical ionization(SPI-CI)combined ion source.By combining capillary sampling technology or molecular beam sampling technology,the applications of VUV-PIMS for real-time and online monitoring of stable products and active intermediates in catalytic processes were introduced,such as ammonia synthesis,methane/ethane catalytic conversion,methanol to olefins.The applications in online monitoring of these catalytic reaction processes exhibited an excellent performance and wide potential applications of VUV-PIMS in process monitoring and reactio

关 键 词：光电离质谱 真空紫外灯 催化反应 活性中间体 在线监测 

分 类 号：O657.63[理学—分析化学]