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Insight into the Activity of Atomically Dispersed Cu Catalysts for Semihydrogenation of Acetylene: Impact of Coordination Environments
Huang, Fei1,2; Peng, Mi3; Chen, Yunlei4,5; Gao, Zirui3; Cai, Xiangbin6; Xie, Jinglin3; Xiao, Dequan7; Jin, Li8; Wang, Guoqing8; Wen, Xiaodong4,9; Wang, Ning6; Zhou, Wu10,11; Liu, Hongyang1,2; Ma, Ding3
Corresponding AuthorLiu, Hongyang(liuhy@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn)
2021-12-09
Source PublicationACS CATALYSIS
ISSN2155-5435
Pages10
AbstractAtomically 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.
Keywordatomically dispersed catalyst Cu catalyst semihydrogenation of acetylene coordination environments structure-performance relationships
Funding OrganizationNational 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
DOI10.1021/acscatal.1c04832
Indexed BySCI
Language英语
Funding ProjectNational 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 Research AreaChemistry
WOS SubjectChemistry, Physical
WOS IDWOS:000731067400001
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:1[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/167320
Collection中国科学院金属研究所
Corresponding AuthorLiu, Hongyang; Ma, Ding
Affiliation1.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
11.Univ Chinese Acad Sci, CAS Key Lab Vacuum Sci, Beijing 100049, Peoples R China
Recommended Citation
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.
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