文献类型：期刊文献

英文题名：Reversibility Iteration Method for Understanding Reaction Networks and for Solving Microkinetics in Heterogeneous Catalysis

作者：Chen, Jian-Fu[1,2];Mao, Yu[3];Wang, Hai-Feng[1,2];Hu, P.[1,2,3]

机构：[1]East China Univ Sci & Technol, Res Inst Ind Catalysis, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Ctr Computat Chem, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland

年份：2016

卷号：6

期号：10

起止页码：7078

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20164202902320);WOS:【SCI-EXPANDED(收录号:WOS:000385057900089)】；

基金：This work was supported by the 973 Program (2013CB933201), the National Natural Science Foundation of China (21333003 and 21303052), the Shanghai Rising-Star Program (14QA1401100) and ChenGuang project (13CG24), Young Elite Scientist Sponsorship Program by CAST and Fundamental Research Funds for the Central Universities. H.-F.W. also thanks the Special Program for Applied Research on Super Computation of the NSFC-Guandong Joint Fund (the second phase) for computing time.

语种：英文

外文关键词：microkinetics; heterogeneous catalysis; reversibility iteration method; turnover frequency; catalytic mechanism; catalysis design

摘要：Solving microkinetics of catalytic systems, which bridges microscopic processes and macroscopic reaction rates, is currently vital for understanding catalysis in silica. However, traditional microkinetic solvers possess several drawbacks that make the process slow and unreliable for complicated catalytic systems. In this paper, a new approach, the so-called reversibility iteration method (RIM), is developed to solve microkinetics for catalytic systems. Using the chemical potential notation we previously proposed to simplify the kinetic framework, the catalytic systems can be analytically illustrated to be logically equivalent to the electric circuit, and the reaction rate and coverage can be calculated by updating the values of reversibilities. Compared to the traditional modified Newton iteration method (NIM), our method is not sensitive to the initial guess of the solution and typically requires fewer iteration steps. Moreover, the method does not require arbitrary-precision arithmetic and has a higher probability of successfully solving the system. These features make it similar to 1000 times faster than the modified Newton iteration method for the systems we tested. Moreover, the derived concept and the mathematical framework presented in this work may provide new insight into catalytic reaction networks.