文献类型：期刊文献

英文题名：Efficient in situ cell modeling boosts catalytic microkinetics quantification by transient infrared spectroscopy

作者：Qiu, Runfa[1];Gu, Haoyuan[1];Li, Didi[2];Jin, Shiqing[1];Gao, Chuang[1];Zhang, Wenhao[1];Jiang, Zhaocong[1];Sun, Bo[1];Cao, Chenxi[3];Zhu, Minghui[1]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Zhengzhou Univ, Coll Chem, Pingyuan Lab, Zhengzhou, Peoples R China;[3]East China Univ Sci & Technol, Key Lab Smart Mfg Energy Chem Proc, Minist Educ, Shanghai, Peoples R China

年份：2025

卷号：71

期号：10

外文期刊名：AICHE JOURNAL

收录：;EI(收录号：20252918817846);WOS:【SCI-EXPANDED(收录号:WOS:001530004300001)】；

基金：Minghui Zhu thanks the research funding sponsored by the National Key R&D Program of China (2022YFB3805504), National Natural Science Foundation of China (22078089), Shanghai Special Program for Fundamental Research (22TQ1400100-7), the Basic Research Program of Science and Technology Commission of Shanghai Municipality (22JC1400600) and SINOPEC (No. 421056). Chenxi Cao acknowledges the funding from the National Natural Science Foundation of China (22441040).

语种：英文

外文关键词：kinetic modeling; MSR; reactor modeling; SSITKA; transient DRIFTS methods

摘要：Operando diffuse reflectance infrared Fourier transform spectroscopy, when combined with transient kinetics approaches, enables quantification of key intermediates and intrinsic kinetics over industrial heterogeneous catalysts. However, these measurements are blurred by residual species within in situ cells due to complex nonideal flow during rapid gas switching. Herein, we model the cell using ideal reactor combinations, with parameters fitted via residence time distribution experiments for two commercial cells by an in-house code. Then, steady-state isotope transient kinetic analysis was conducted for methanol steam reforming to derive rate constants for crucial surface reactions. Our approach estimated microkinetic parameters precisely and consistently across both cell designs, prevailing over conventional methods that produced inconsistent results. This analytical framework not only boosts the effectiveness of existing in situ cells in catalytic process development, but also lays a critical foundation for the design and optimization of next-generation spectroscopic systems.