Insight into the Activity of Atomically Dispersed Cu Catalysts for Semihydrogenation of Acetylene: Impact of Coordination Environments

doi:10.1021/acscatal.1c04832

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	Insight into the Activity of Atomically Dispersed Cu Catalysts for Semihydrogenation of Acetylene: Impact of Coordination Environments
	Huang, Fei 1,2; Peng, Mi 3; Chen, Yunlei 4,5; Gao, Zirui 3; Cai, Xiangbin 6; Xie, Jinglin 3; Xiao, Dequan 7; Jin, Li 8; Wang, Guoqing 8; Wen, Xiaodong 4,9
刊名	ACS CATALYSIS
	2021-12-09
页码	10
关键词	atomically dispersed catalyst Cu catalyst semihydrogenation of acetylene coordination environments structure-performance relationships
ISSN号	2155-5435
DOI	10.1021/acscatal.1c04832
通讯作者	Liu, Hongyang(liuhy@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn)
英文摘要	Atomically dispersed metal catalysts (ADMCs), which offer maximized atom-use efficiency and catalytic perform-ance enhancements for many catalytic systems, have received increasing attention in the catalysis field. Additionally, ADMCs with well-defined architectures are promising for providing valuable information to derive structure-performance relation-ships. Here, we immobilized Cu1 on a defective nanodiamond-graphene (ND@G) and N-doped nanodiamond-graphene (ND@ NG). By changing the coordination environments (Cu-C or Cu-N), the electronic state of Cu ADMCs can be tailored. The highly oxidized Cu atoms in Cu-N AMDCs present distinctively different acetylene hydrogenation activity compared to that in Cu-C AMDCs (i.e., with high conversion (100%), high selectivity (93%), and good stability (more than for 100 h)). Density functional theory and H-2-D-2 exchange experiments reveal that Cu-C bond anchoring favors H-2 dissociative adsorption, which is a rate-limiting step. In addition, the facile desorption of the target product C2H4 over Cu-C ADMCs ensures the outstanding activity and selectivity of the catalyst. This work thus helps to bring perspectives for linking activity and structures of ADMCs and designing active ADMCs for hydrogenation applications.
资助项目	National Key R&D Program of China[2016YFA0204100] ; National Key R&D Program of China[2017YFB0602200] ; National Natural Science Foundation of China[21961160722] ; National Natural Science Foundation of China[22072162] ; National Natural Science Foundation of China[91845201] ; National Natural Science Foundation of China[21725301] ; National Natural Science Foundation of China[91645115] ; National Natural Science Foundation of China[21821004] ; Liaoning Revitalization Talents Program[XLYC1907055] ; Dalian National Lab for Clean Energy (DNL Cooperation Fund)[202001] ; China Petroleum & Chemical Corporation[420043-2] ; Research Grants Council of Hong Kong[16306818] ; Research Grants Council of Hong Kong[C6021-14E]
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000731067400001
资助机构	National Key R&D Program of China ; National Natural Science Foundation of China ; Liaoning Revitalization Talents Program ; Dalian National Lab for Clean Energy (DNL Cooperation Fund) ; China Petroleum & Chemical Corporation ; Research Grants Council of Hong Kong
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/167319]
专题	金属研究所_中国科学院金属研究所
通讯作者	Liu, Hongyang; Ma, Ding
作者单位	1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 2.Univ Sci & Technol China, Sch Mat Sci & Engn, Hefei 230026, Peoples R China 3.Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Engn, Beijing 100871, Peoples R China 4.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China 5.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 6.Hong Kong Univ Sci & Technol, Dept Phys, Kowloon, Hong Kong, Peoples R China 7.Univ New Haven, Ctr Integrat Mat Discovery, Dept Chem & Chem Engn, West Haven, CT 06516 USA 8.Sinopec Beijing Res Inst Chem Ind, Beijing 100013, Peoples R China 9.Synfuels China Co Ltd, Natl Energy Ctr Coal Clean Fuel, Beijing 100871, Peoples R China 10.Univ Chinese Acad Sci, Sch Phys Sci, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Huang, Fei,Peng, Mi,Chen, Yunlei,et al. Insight into the Activity of Atomically Dispersed Cu Catalysts for Semihydrogenation of Acetylene: Impact of Coordination Environments[J]. ACS CATALYSIS,2021:10.
APA	Huang, Fei.,Peng, Mi.,Chen, Yunlei.,Gao, Zirui.,Cai, Xiangbin.,...&Ma, Ding.(2021).Insight into the Activity of Atomically Dispersed Cu Catalysts for Semihydrogenation of Acetylene: Impact of Coordination Environments.ACS CATALYSIS,10.
MLA	Huang, Fei,et al."Insight into the Activity of Atomically Dispersed Cu Catalysts for Semihydrogenation of Acetylene: Impact of Coordination Environments".ACS CATALYSIS (2021):10.