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通过质谱测量进行现场反应监测和机制研究:异质光催化和初始接触反应

Qixin Tang¹, Cunhao Cui^1,2, Haotian Ying¹

¹State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, P.R. China.

Analytical chemistry

|August 15, 2025

概括

本研究引入了一种"源内反应"方法,用于实时跟踪催化表面过程. 该技术使用集成的反应器和电喷气电离源来检测过渡物种,推进异质催化研究.

科学领域:

不同质的催化剂.
表面化学表面化学
分析化学分析化学

背景情况:

在异质催化中阐明反应机制需要实时跟踪固体-液体界面的短暂物种.
传统的质谱 (MS) 在直接探测表面过程中面临局限性.
需要先进的技术来监测高时间分辨率的表面反应.

研究的目的:

开发一种创新的"源内反应"战略,将微反应器与电喷离子化 (ESI) 源相结合.
为了能够直接,次秒分辨率检测从催化面上脱落的物种.
提供一种敏感且可行的方法,用于追踪液体-固体异质催化反应中的表面过程.

主要方法:

各种催化剂 (g-C3N4,TiO2,化物,Pd/C) 在玻璃探针 (GP) 中被固定.
在GP作为一个集成的微反应器和ESI源直接物种检测.
使用现场监测来追踪光催化降解和素转化反应.

主要成果:

检测到Brilliant Green (BG) 光催化降解中的40多种中间体,揭示了g-C3N4和TiO2.2的独特机制.
该方法成功追踪了BG和其他染料的光催化降解.
在素模型化合物转换过程中,观察到表面吸附的GGGE在Pd上的脱水和在支表面上的自发循环.

结论:

开发的"源内反应"策略提供了一种新,可行和敏感的方法,用于跟踪异质催化中的表面过程.
这种方法克服了用于探测固体-液体接口的传统MS的局限性.
该技术在各种催化反应系统中具有广泛的适用性.

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