Cooperative Sites in Fully Exposed Pd Clusters for Low-Temperature Direct Dehydrogenation Reaction | |
Wang, Linlin1,2; Diao, Jiangyong2; Peng, Mi3,4; Chen, Yunlei5; Cai, Xiangbin6; Deng, Yuchen3,4; Huang, Fei2; Qin, Xuetao3,4; Xiao, Dequan7; Jiang, Zheng8; Wang, Ning6; Sun, Ting1; Wen, Xiaodong5; Liu, Hongyang2; Ma, Ding3,4 | |
Corresponding Author | Wen, Xiaodong(wxd@sxicc.ac.cn) ; Liu, Hongyang(liuhy@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn) |
2021-09-17 | |
Source Publication | ACS CATALYSIS
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ISSN | 2155-5435 |
Volume | 11Issue:18Pages:11469-11477 |
Abstract | Direct dehydrogenation of alkanes is of great interest but presents a significant challenge in activating C-H bond at a low temperature. Here, we report fully exposed Pd clusters consisting of an average of three Pd atoms on a hybrid nanodiamond-graphene support (denoted as Pd-3/ND@G) for low-temperature dehydrogenation of ethylbenzene to styrene. The obtained fully exposed and atomically dispersed Pd clusters exhibit good catalytic performance (328 mmol g(Pd)(-1) h(-1) ethylbenzene conversion rate and >99% styrene selectivity) and much enhanced stability under oxygen-free conditions at 350 degrees C, compared with the previously reported catalysts. The synergetic interaction between adjacent Pd atoms in each cluster evidenced by density functional theory (DFT) calculations guarantees effective activation of C-H bond on ethyl in ethylbenzene and easy desorption of styrene, which is the key for the higher activity than typical Pd single atom and Pd nanoparticle catalysts. The present method for precise control of fully exposed Pd clusters paves a new way for designing direct dehydrogenation catalyst at the atomic scale. |
Keyword | atomic dispersion Pd cluster defect-rich graphene dehydrogenation heterogeneous catalysis |
Funding Organization | Ministry of Science and Technology ; National Natural Science Foundation of China ; Dalian National Lab for Clean Energy, DNL Cooperation Fund, CAS ; Liaoning Revitalization Talents Program ; Sinopec China ; Research Grants Council of Hong Kong |
DOI | 10.1021/acscatal.1c01503 |
Indexed By | SCI |
Language | 英语 |
Funding Project | Ministry of Science and Technology[2016YFA0204100] ; Ministry of Science and Technology[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[21703261] ; National Natural Science Foundation of China[21725301] ; National Natural Science Foundation of China[91645115] ; National Natural Science Foundation of China[21821004] ; Dalian National Lab for Clean Energy, DNL Cooperation Fund, CAS[202001] ; Liaoning Revitalization Talents Program[XLYC1907055] ; Sinopec China ; Research Grants Council of Hong Kong[C6021-14E] ; Research Grants Council of Hong Kong[N_HKUST624/19] ; Research Grants Council of Hong Kong[16306818] |
WOS Research Area | Chemistry |
WOS Subject | Chemistry, Physical |
WOS ID | WOS:000697346200014 |
Publisher | AMER CHEMICAL SOC |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.imr.ac.cn/handle/321006/167020 |
Collection | 中国科学院金属研究所 |
Corresponding Author | Wen, Xiaodong; Liu, Hongyang; Ma, Ding |
Affiliation | 1.Northeastern Univ, Dept Chem, Shenyang 110819, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Engn, Beijing 100871, Peoples R China 4.Peking Univ, Coll Engn, BIC ESAT, Beijing 100871, Peoples R China 5.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, 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.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China |
Recommended Citation GB/T 7714 | Wang, Linlin,Diao, Jiangyong,Peng, Mi,et al. Cooperative Sites in Fully Exposed Pd Clusters for Low-Temperature Direct Dehydrogenation Reaction[J]. ACS CATALYSIS,2021,11(18):11469-11477. |
APA | Wang, Linlin.,Diao, Jiangyong.,Peng, Mi.,Chen, Yunlei.,Cai, Xiangbin.,...&Ma, Ding.(2021).Cooperative Sites in Fully Exposed Pd Clusters for Low-Temperature Direct Dehydrogenation Reaction.ACS CATALYSIS,11(18),11469-11477. |
MLA | Wang, Linlin,et al."Cooperative Sites in Fully Exposed Pd Clusters for Low-Temperature Direct Dehydrogenation Reaction".ACS CATALYSIS 11.18(2021):11469-11477. |
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