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A Magnetically Separable Pd Single-Atom Catalyst for Efficient Selective Hydrogenation of Phenylacetylene
Zhao, Linmin1,2; Qin, Xuetao3,4,5; Zhang, Xirui6; Cai, Xiangbin7,8; Huang, Fei1,2; Jia, Zhimin1,2; Diao, Jiangyong1,2; Xiao, Dequan9; Jiang, Zheng10; Lu, Ruifeng6; Wang, Ning7,8; Liu, Hongyang1,2; Ma, Ding3,4,5
通讯作者Liu, Hongyang(liuhy@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn)
2022-04-15
发表期刊ADVANCED MATERIALS
ISSN0935-9648
页码8
摘要Selective hydrogenation of alkynes to alkenes plays a crucial role in the synthesis of fine chemicals. However, how to achieve high selectivity and effective separation of the catalyst and substrate while obtaining high activity is the key for this reaction. In this work, a Pd single-atom catalyst is anchored to the shell of magnetic core-shell particles that consist of a Ni-nanoparticles core and a graphene sheets shell (Ni@G) for semi-hydrogenation of phenylacetylene, delivering 93% selectivity to styrene at full conversion with a robust turnover frequency of 7074 h(-1) under mild reaction conditions (303 K, 2 bar H-2). Moreover, the catalyst can be recovered promptly from the liquid phase due to its magnetic separability, which makes it present good stability for enduring five cycles. Experimental and theoretical investigations reveal that H-2 and substrates are activated by atomically dispersed Pd atoms and Ni@G hybrid support, respectively. The hydrogenation reaction occurs on the surface of Ni@G via hydrogen spillover from the metal to the support. Such a strategy opens an avenue for designing highly active, selective, and magnetically recyclable catalysts for selective hydrogenation in liquid reaction systems.
关键词heterogeneous catalysis magnetically separable catalysts palladium single-atom catalysts selective hydrogenation reaction
资助者National Key R&D Program of China ; National Natural Science Foundation of China ; Liaoning Revitalization Talents Program ; Natural Science Foundation of Liaoning Province ; Dalian National Lab for Clean Energy (DNL Cooperation Fund) ; Sinopec China ; Research Grants Council of Hong Kong
DOI10.1002/adma.202110455
收录类别SCI
语种英语
资助项目National Key R&D Program of China[2016YFA0204100] ; National Key R&D Program of China[2021YFA1501100] ; National Natural Science Foundation of China[U21B2092] ; National Natural Science Foundation of China[91845201] ; National Natural Science Foundation of China[21961160722] ; National Natural Science Foundation of China[22072162] ; 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] ; Natural Science Foundation of Liaoning Province[2021-MS-001] ; Dalian National Lab for Clean Energy (DNL Cooperation Fund)[202001] ; 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研究方向Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS类目Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS记录号WOS:000782671200001
出版者WILEY-V C H VERLAG GMBH
引用统计
被引频次:82[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/172792
专题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 Sci, Beijing 100871, Peoples R China
4.Peking Univ, Coll Engn, Beijing 100871, Peoples R China
5.Peking Univ, BIC ESAT, Beijing 100871, Peoples R China
6.Nanjing Univ Sci & Technol, Dept Appl Phys, Nanjing 210094, Peoples R China
7.Hong Kong Univ Sci & Technol, Dept Phys, Kowloon, Clear Water Bay, Hong Kong, Peoples R China
8.Hong Kong Univ Sci & Technol, Ctr Quantum Mat, Kowloon, Clear Water Bay, Hong Kong, Peoples R China
9.Univ New Haven, Dept Chem & Chem & Biomed Engn, Ctr Integrat Mat Discovery, 300 Boston Post Rd, West Haven, CT 06516 USA
10.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201204, Peoples R China
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GB/T 7714
Zhao, Linmin,Qin, Xuetao,Zhang, Xirui,et al. A Magnetically Separable Pd Single-Atom Catalyst for Efficient Selective Hydrogenation of Phenylacetylene[J]. ADVANCED MATERIALS,2022:8.
APA Zhao, Linmin.,Qin, Xuetao.,Zhang, Xirui.,Cai, Xiangbin.,Huang, Fei.,...&Ma, Ding.(2022).A Magnetically Separable Pd Single-Atom Catalyst for Efficient Selective Hydrogenation of Phenylacetylene.ADVANCED MATERIALS,8.
MLA Zhao, Linmin,et al."A Magnetically Separable Pd Single-Atom Catalyst for Efficient Selective Hydrogenation of Phenylacetylene".ADVANCED MATERIALS (2022):8.
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