文献类型：期刊文献

英文题名：Correlation between the structural features and intrinsic activity trend of Fe surfaces for ammonia synthesis

作者：Chen, Jianfu[1,2];Chen, Ye[1,2];Wang, Haifeng[1,2];Hu, P.[3,4]

机构：[1]East China Univ Sci & Technol, Ctr Computat Chem, State Key Lab Green Chem Engn & Ind Catalysis, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci andTechnol, Res Inst Ind Catalysis, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]ShanghaiTech Univ, Sch Phys Sci & Technol, 393 Middle Huaxia Rd, Shanghai 201210, Peoples R China;[4]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, North Ireland

年份：2023

卷号：13

期号：18

起止页码：5237

外文期刊名：CATALYSIS SCIENCE & TECHNOLOGY

收录：;EI(收录号：20233614681099);WOS:【SCI-EXPANDED(收录号:WOS:001048893900001)】；

基金：NSFC (92045303, 21703067, 22202069, 21873028) and NKRDPC (2021YFA1500700) are acknowledged.

语种：英文

外文关键词：Ammonia - Catalyst activity - Density functional theory

摘要：The Haber-Bosch process, which was developed more than a century ago, remains the primary method for nitrogen fixation on a large scale and Fe is typically the main catalyst used in the process. Despite having been extensively studied, some anomalies regarding the activity trend across various Fe surfaces still exist. To understand the intrinsic activity trend of Fe catalysts, we utilize density functional theory (DFT) to calculate the reaction energetics on various Fe surfaces in conjunction with microkinetic analyses to examine the activity of the Fe surfaces. The catalytic activity order obtained is Fe(111) > Fe(211) > Fe(210) > Fe(100) > Fe(110). We find that the activity trend is correlated to the barrier of the rate-determining step, N-2 dissociative adsorption barrier, and perhaps more importantly to the surface energies. It is also noted that the association barriers of flat surfaces are generally larger than those of stepped surfaces, for which a clear explanation is provided.