文献类型：期刊文献

英文题名：Reaction mechanism of CO activation and methane formation on Co Fischer-Tropsch catalyst: A combined DFT, transient, and steady-state kinetic modeling

作者：Yang, Jia[1];Qi, Yanying[1];Zhu, Jun[1];Zhu, Yi-An[2];Chen, De[1];Holmen, Anders[1]

机构：[1]Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway;[2]E China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China

年份：2013

卷号：308

起止页码：37

外文期刊名：JOURNAL OF CATALYSIS

收录：;EI(收录号：20135017070060);WOS:【SCI-EXPANDED(收录号:WOS:000329881700005)】；

基金：Dr. Zhixin Yu is greatly acknowledged for providing the catalyst. The financial support from The Norwegian Research Council through the KOSK program and the Norwegian University of Science and Technology is gratefully acknowledged.

语种：英文

外文关键词：Fischer-Tropsch; Methanation; Transient kinetics; Cobalt catalysts

摘要：A new approach for elucidating reaction mechanism of complex reactions, such as Fischer-Tropsch (F-T) synthesis, is presented. It includes a combination of integrated transient and steady-state kinetic modeling, experimental and DFT investigations of kinetic isotopic effects. The integrated transient and steady-state modeling enable the determination of H-2 and CO equilibrium constants and detailed mapping of surface species including surface concentrations and their reactivities. The predictive ability of Langmuir-Hinshelwood type kinetic models has been significantly improved by taking into account the effect of interaction between adsorbed CO on the CO adsorption. Together with DFT investigations of the kinetic isotopic effect, the dominating CO activation pathway through hydrogen-assisted CO dissociation has been confirmed. It led also to a clarification of two carbon pools namely CH2O* (C alpha) and CHx* (C beta) and two corresponding reaction pathways for methane formation. The prevailing reaction pathway for methane formation depends on the operating conditions. Hydrogen surface concentration is the key parameter determining the reactivity of adsorbed CO and the reaction pathways for methane formation. (C) 2013 Elsevier Inc. All rights reserved.