文献类型：期刊文献

中文题名：Mechanistic aspects of facet-dependent CH_(4)/C_(2+)selectivity over aχ-Fe_(5)C_(2)Fischer-Tropsch catalyst

作者：Thanh Hai Pham[1,2];Junbo Cao[1];Nan Song[1];Yueqiang Cao[1];Bingxu Chen[1];Gang Qian[1];Xinggui Zhou[1];De Chen[3];Xuezhi Duan[1]

机构：[1]State Key Laboratory of Chemical Engineering,East China University of Science and Technology,130 Meilong Road,Shanghai,200237,China;[2]Vietnam Institute for Tropical Technology and Environmental Protection,57A Truong Quoc Dung,Ho Chi Minh,Viet Nam;[3]Department of Chemical Engineering,Norwegian University of Science and Technology,N-7491,Trondheim,Norway

年份：2022

卷号：7

期号：3

起止页码：449

中文期刊名：Green Energy & Environment

外文期刊名：绿色能源与环境（英文版）

收录：CSTPCD;;Scopus;CSCD:【CSCD2021_2022】；

基金：financially supported by the Natural Science Foundation of China(21922803 and 21776077);the Program for the Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning;the State Key Laboratory of Organic-Inorganic Composites(oic-201801007);the Open Project of State Key Laboratory of Chemical Engineering(SKLChe-15C03)。

语种：英文

中文关键词：selectivity;catalyst;coupling;

摘要：Structure-performance relationship is a complex issue in iron-catalyzed Fischer-Tropsch synthesis,and it is not easy to elucidate it by experimental investigations.First-principle calculation is a powerful method for explaining experimental results and guiding catalyst design.In this study,we investigated the reaction mechanisms of CH_(4)formation and C-C coupling on fourχ-Fe_(5)C_(2)surfaces and established the kinetic equations to compare the rates of CH_(4)formation and C_(1)+C_(1)coupling reactions and determine the CH_(4)/C_(2+)selectivity.The results show that the geometry of theχ-Fe_(5)C_(2)surfaces has little effect on the formation rate of CH_(4);however,the C_(1)+C_(1)coupling reactions are significantly affected by the surface geometry.The C_(1)+C_(1)coupling reaction rates on the terraced-like(510)and(021)surfaces are much higher than those on the stepped-like(001)and(100)surfaces.Based on these results,we established a Brùnsted-Evans-Polanyi(BEP)relationship between the effective barrier difference for CH_(4)formation and C_(1)+C_(1)coupling(ΔE_(eff))and the adsorption energy of C+4H(ΔE_(C+4H))onχ-Fe_(5)C_(2)surfaces.ΔE_(C+4H)can be used as a descriptor for CH_(4)/C_(2+)selectivity on different surfaces ofχ-Fe_(5)C_(2).