Surface modification of Fe5C2 by binding silica-based ligand: A theoretical explanation of enhanced C2 oxygenate selectivity

doi:10.1016/j.mcat.2023.113333

IMECH-IR > 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
	Yin, Junqing ; Wang, Shuyuan ; Xu, Dan ; You, Yong ; Liu, Xingchen ; Peng Q(彭庆)
发表期刊	MOLECULAR CATALYSIS
	2023-08-01
卷号	547 页码:113333
ISSN	2468-8231
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.
关键词	Surface modification Iron carbide Support -like ligand Catalytic selectivity Fischer-Tropsch Synthesis
DOI	10.1016/j.mcat.2023.113333
收录类别	SCI ; EI
语种	英语
WOS记录号	WOS:001032319200001
WOS研究方向	Chemistry
WOS类目	Chemistry, Physical
项目资助者	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.
论文分区	二类
力学所作者排名	3+
RpAuthor	Yin, JQ (corresponding author), Chengdu Univ, Inst Adv Study, Chengdu 610106, Peoples R China.
引用统计	被引频次：3[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://dspace.imech.ac.cn/handle/311007/92612
专题	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.

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