State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
Institute of Engineering Technology, SINOPEC Catalyst Co., Ltd., Beijing, 110112, P. R. China.
Chemistry. 2023 Apr 25;29(24):e202203781. doi: 10.1002/chem.202203781. Epub 2023 Mar 20.
Water-gas shift (WGS) reaction offers a dominating path to hydrogen generation from fossil fuel, in which heterogeneous metal catalysts play a crucial part in this course. This review highlights and summarizes recent developments on theoretical calculations of metal catalysts developed to date, including surface structure (e. g., monometallic and polymetallic systems) and interface structure (e. g., supported catalysts and metal oxide composites), with special emphasis on the characteristics of crystal-face effect, alloying strategy, and metal-support interaction. A systematic summarization on reaction mechanism was performed, including redox mechanism, associative mechanism as well as hybrid mechanism; the development on chemical kinetics (e. g., molecular dynamics, kinetic Monte Carlo and microkinetic simulation) was then introduced. At the end, challenges associated with theoretical calculations on metal catalysts toward WGS reaction are discussed and some perspectives on the future advance of this field are provided.
水汽变换（WGS）反应为化石燃料制氢提供了主要途径，其中多相金属催化剂在这一过程中起着至关重要的作用。本综述重点介绍并总结了迄今为止针对金属催化剂的理论计算方面的最新进展，包括表面结构（例如单金属和多金属体系）和界面结构（例如负载型催化剂和金属氧化物复合材料），特别强调了晶面效应、合金化策略和金属-载体相互作用的特点。对反应机制进行了系统总结，包括氧化还原机制、缔合机制以及混合机制；随后介绍了化学动力学的发展（例如分子动力学、动力学蒙特卡罗和微动力学模拟）。最后，讨论了与 WGS 反应金属催化剂理论计算相关的挑战，并对该领域的未来发展提出了一些看法。
