文献类型：期刊文献

英文题名：Possible Strong Promotional Effect of Al2O3 on Fe Catalysts for Ammonia Synthesis via Fe/γ-Al2O3

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

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

年份：2025

卷号：15

期号：15

起止页码：13366

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20253318984637);WOS:【SCI-EXPANDED(收录号:WOS:001532359200001)】；

基金：NSFC (22473043, 92045303) and NKRDPC (2021YFA1500700) are acknowledged.

语种：英文

外文关键词：ammonia synthesis; gamma-Al2O3; Fe-based catalyst; DFT; molecular dynamics; micro-kinetic analyses

摘要：Al2O3 is a critical component in Fe-based catalysts for ammonia synthesis, yet its precise promotional role remains elusive. In this work, we employ density functional theory (DFT) and molecular dynamics (MD) simulations to investigate the catalytic behavior of Fe surfaces supported on gamma-Al2O3, the most common phase of Al2O3 used as a support. A series of Fe(110)/gamma-Al2O3 models with varying Fe layer thicknesses are constructed, in which the Fe(110) facet is typically the least active among Fe surfaces. Reaction energies and activation barriers are computed for each system, followed by microkinetic simulations based on the calculated energetics. The results reveal a pronounced promotional effect of gamma-Al2O3: Its interaction with Fe(110) significantly lowers the barrier for N-2 dissociative adsorption, elevating the predicted catalytic activity to a level comparable with that of Fe(111), the most active Fe surface. Structural analysis further shows that monolayer Fe(110)/gamma-Al2O3 closely resembles the geometry of stepped Fe surfaces. As the number of Fe layers increases, the structural distortion induced by gamma-Al2O3 diminishes, and the system gradually reverts to the characteristics of pristine Fe(110).