文献类型：期刊文献

英文题名：Examination of the key issues in microkinetics: CO oxidation on Rh(111)

作者：Guo, Chenxi[1];Mao, Yu[1];Yao, Zihao[1];Chen, Jianfu[2,3];Hu, P.[1]

机构：[1]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland;[2]East China Univ Sci & Technol, Key Lab Adv Mat, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Ctr Computat Chem, Shanghai 200237, Peoples R China

年份：2019

卷号：379

起止页码：52

外文期刊名：JOURNAL OF CATALYSIS

收录：;EI(收录号：20194007489390);WOS:【SCI-EXPANDED(收录号:WOS:000497249700007)】；

基金：UK Archer and QUB Kelvin provides supercomputing service. C.X.G. thanks the Queen's University of Belfast and China Scholarship Council for finance support. National Natural Science Foundation of China (21333003, 201703067) is acknowledged. J.F.C. thanks Postdoctoral Science Foundation of China (2017M611471).

语种：英文

外文关键词：CO oxidation; Adsorbate-adsorbate interactions; Microkinetic modeling

摘要：Microkinetic modelling plays the key role to bridge first principles calculations at the atomic level to experimental data at macroscopic scales. Currently, some significant differences between the microkinetic modelling results and experimental ones still exist. In this work, CO oxidation on Rh(111) is selected as a model system for its simplicity as well as its importance, and an in-depth study of microkinetic modelling on the reaction is performed. A self-consistent microkinetic modelling iterating with respect to coverages is developed. It is found that a good accuracy of the microkinetic modelling using density functional theory energies can be obtained if adsorbate-adsorbate interactions including the coverage effect on the transition states are rigorously calculated. The calculated kinetic results including the turnover frequency (TOF), which are very close to experimental ones, can be achieved if corrections of the over-estimation of chemisorption energies of density functional theory and van der Waals forces are also included. (C) 2019 Elsevier Inc. All rights reserved.