中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
首页 机构 成果 学者
  
  1. CAS IR Grid
  2. 力学研究所
  3. 中国科学院力学研究所
  4. 非线性力学国家重点实验室
Surface modification of Fe5C2 by binding silica-based ligand: A theoretical explanation of enhanced C2 oxygenate selectivity

文献类型：期刊论文

作者Yin, Junqing; Wang, Shuyuan; Xu, Dan; You, Yong; Liu, Xingchen; Peng Q(彭庆)
刊名MOLECULAR CATALYSIS
出版日期2023-08-01
卷号547页码:113333
ISSN号2468-8231
关键词Surface modification Iron carbide Support -like ligand Catalytic selectivity Fischer-Tropsch Synthesis
DOI10.1016/j.mcat.2023.113333
英文摘要Elucidating the role(s) of support-like ligands remains a challenge in catalytic reaction like the Fischer-Tropsch Synthesis (FTS) catalyzed by the iron catalyst supported on silica. We herein theoretically investigated surface modification of Fe5C2 by silica-based ligand and its influence on C2 oxygenate selectivity in FTS, by carrying out DFT calculations on dissociation of CO and formations of CH4 and C2 on ha-SiO2/Fe5C2(510). To mimic the structure of surface modification, the ha-SiO2/Fe5C2(510) model was built up by binding the silica cluster (the ha-SiO2 ligand) to Fe5C2(510). DFT calculations elucidated that the C + CH coupling with the lowest activation barrier among all the possible routes of C2 formation on Fe5C2(510) is suppressed after modification with the haSiO2 ligand because the binding ha-SiO2 ligand limits the geometry relaxation caused by the C+CH coupling. However, CO molecule is anchored by the ha-SiO2 ligand via hydrogen bond, suppressing the C-O cleavage because the d-valence band center of Fe5C2(510) lowers in energy by surface modification with the ha-SiO2 ligand, but facilitating the C + CO coupling with the lowest activation barrier among all the possible routes of C2 formation. Also, CH4 formation in the ha-SiO2/Fe5C2(510) case is not so easy as that on Fe5C2(510). Therefore, C2 oxygenate is formed more easily in the ha-SiO2/Fe5C2(510) case than in the Fe5C2(510) case. The result agrees with the experimental observation that C2 oxygenate selectivity became high for iron-based FTS catalyst after surface modification of by silica-based ligand.
分类号二类
WOS研究方向Chemistry
语种英语
WOS记录号WOS:001032319200001
资助机构Natural Science Foundation of Sichuan Province [2023NSFSC1080] ; Talent Program of Chengdu University [2081923010] ; Qilu University of Technology (Shandong Academy of Sciences) Project [2022JBZ02-03] ; Synfuels China Co. Ltd.
其他责任者Yin, JQ (corresponding author), Chengdu Univ, Inst Adv Study, Chengdu 610106, Peoples R China.
源URL[http://dspace.imech.ac.cn/handle/311007/92612]  
专题力学研究所_非线性力学国家重点实验室
作者单位1.{Yin, Junqing, You, Yong} Chengdu Univ, Inst Adv Study, Chengdu 610106, Peoples R China
2.{Wang, Shuyuan, Xu, Dan} Qilu Univ Technol, Energy Res Inst, Sch Energy & Power Engn, Jinan 250014, Peoples R China
3.{Yin, Junqing} Synfuels China Co Ltd, Natl Energy Canter Coal Liquids, Beijing 101400, Peoples R China
4.{Liu, Xingchen} Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
5.{Peng, Qing} Chinese Acad Sci, Inst Mech, State Key Lab Nonlinear Mech, Beijing 100190, Peoples R China
推荐引用方式
GB/T 7714		 Yin, Junqing,Wang, Shuyuan,Xu, Dan,et al. Surface modification of Fe5C2 by binding silica-based ligand: A theoretical explanation of enhanced C2 oxygenate selectivity[J]. MOLECULAR CATALYSIS,2023,547:113333.
APA Yin, Junqing,Wang, Shuyuan,Xu, Dan,You, Yong,Liu, Xingchen,&彭庆.(2023).Surface modification of Fe5C2 by binding silica-based ligand: A theoretical explanation of enhanced C2 oxygenate selectivity.MOLECULAR CATALYSIS,547,113333.
MLA Yin, Junqing,et al."Surface modification of Fe5C2 by binding silica-based ligand: A theoretical explanation of enhanced C2 oxygenate selectivity".MOLECULAR CATALYSIS 547(2023):113333.

入库方式： OAI收割

来源：力学研究所

浏览0
下载0
收藏0
其他版本

除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。