CO hydrogenation conversion driven by micro-environments of active sites over iron carbide catalysts  

作　　者：Nan Song Xingxing Li Ebtihal Abograin Wenyao Chen Junbo Cao Jing Zhang De Chen Xuezhi Duan Xinggui Zhou 

机构地区：[1]State Key Laboratory of Chemical Engineering,East China University of Science and Technology,130 Meilong Road,Shanghai,200237,China [2]Department of Chemical Engineering,Norwegian University of Science and Technology,Trondheim,7491,Norway

出　　处：《Green Energy & Environment》2025年第2期367-373,共7页绿色能源与环境(英文版)

基　　金：supported by the Research Fund for National Key Research and Development Program of China(2022YFA1503804,2021YFA1501403);the Natural Science Foundation of China(22208094,21922803,92034301,22008066 and 21776077);the China Postdoctoral Science Foundation(BX20190116);the Innovation Program of Shanghai Municipal Education Commission(17ZR1407300);the Program of Shanghai Academic/Technology Research Leader(21XD1421000).

摘　　要：Essentially clearing the structure-activity relationship between iron carbide catalysts involving multiple active centers to understand the reaction mechanism of CO hydrogenation conversion process is still a great challenge.Here,two main micro-environment factors,namely electronic properties and geometrical effects were found to have an integrated effect on the mechanism of CO hydrogenation conversion,involving active sites on multiple crystal phases.The Bader charge of the surface Fe atoms on the active sites had a guiding effect on the CO activation pathway,while the spatial configuration of the active sites greatly affected the energy barriers of CO activation.Although the defective surfaces were more conducive to CO activation,the defective sites were not the only sites to dissociate CO,as CO always tended to dissociate in a wider area.This synergistic effect of the micro-environment also occurred during the CO conversion process.Surface C atoms on relatively flat configurations were more likely to form methane,while the electronic properties of the active sites could effectively describe the C-C coupling process,as well as distinguish the coupling mechanisms.

关 键 词：MICRO-ENVIRONMENT CO hydrogenation conversion Electronic property Local environment Synergistic effect 

分 类 号：O643.36[理学—物理化学] X701[理学—化学]