文献类型：期刊文献

英文题名：CO hydrogenation conversion driven by micro-environments of active sites over iron carbide catalysts

作者：Song, Nan[1];Li, Xingxing[1];Abograin, Ebtihal[1];Chen, Wenyao[1];Cao, Junbo[1];Zhang, Jing[1];Chen, De[2];Duan, Xuezhi[1];Zhou, Xinggui[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway

年份：2025

卷号：10

期号：2

起止页码：367

外文期刊名：GREEN ENERGY & ENVIRONMENT

收录：;EI(收录号：20241415837125);WOS:【SCI-EXPANDED(收录号:WOS:001447636600001)】；

基金：This work was financially 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) .

语种：英文

外文关键词：Micro-environment; CO hydrogenation conversion; Electronic property; Local environment; Synergistic effect

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. (c) 2024 Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co., Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).