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Fully Exposed Nickel Clusters for Semihydrogenation of Acetylene

文献类型：期刊论文

作者Sui, Chengquan1,2; Ma, Huan3,4,5; Huang, Fei1,6; Wang, Maolin7; Cai, Xiangbin8,9; Diao, Jiangyong1; Ren, Pengju4,5; Wen, Xiaodong4,5; Jin, Li10; Wang, Guoqing10
刊名ACS CATALYSIS
出版日期2024-09-19
卷号14期号:19页码:14689-14695
关键词semihydrogenation reaction non-noble metalcatalyst atomically dispersed metal catalyst fullyexposed cluster acetylene
ISSN号2155-5435
DOI10.1021/acscatal.4c04462
通讯作者Wang, Guoqing(Wanggq.bjhy@sinopec.com) ; Ma, Ding(dma@pku.edu.cn) ; Liu, Hongyang(liuhy@imr.ac.cn)
英文摘要Semihydrogenation of acetylene to ethylene is a key process for ethylene purification in the chemical industry. The pursuit of an effective non-noble metal acetylene selective hydrogenation catalyst with low cost, high efficiency, and ultrastability is extremely urgent, especially for industrial applications. However, achieving high ethylene selectivity at full conversion under a low reaction temperature remains challenging due to the imbalance of the H-2 splitting ability and intermediate (ethylene) hydrogenation. Herein, we designed atomically dispersed and fully exposed Ni clusters on a nanodiamond@graphene support. H-2-D-2 exchange experiments and density functional theory calculations reveal that acetylene and hydrogen can be efficiently activated on fully exposed Ni cluster sites due to the enhanced catalytic hydrogenation catalytic ability. Furthermore, the desorption of ethylene on fully exposed Ni cluster sites is much more favored compared to further dissociation of H-2, leading to the high selectivity of ethylene. Thereby, the fully exposed Ni cluster catalyst delivered an ethylene selectivity of 85% at full conversion for semihydrogenation of acetylene at 190 degree celsius with a specific activity of 667 mL(C2H2)g(Ni)(-1)min(-1), exceeding the catalytic efficiency of most supported Ni catalysts. The implementation of the fully exposed Ni cluster catalyst provides an effective strategy for improving the catalytic efficiency of non-noble metal acetylene selective hydrogenation catalysts while obtaining high ethylene selectivity. The precise regulation of metal active sites at the subnanometer scale has a significant effect on the rational design of high catalytic performance atomically dispersed non-noble metal catalysts.
资助项目National Key R&D Program of China[2022YFB4003100] ; National Key R&D Program of China[2022YFA1504500] ; National Natural Science Foundation of China[22202213] ; National Natural Science Foundation of China[22072162] ; National Natural Science Foundation of China[92145301] ; National Natural Science Foundation of China[U21B2092] ; National Natural Science Foundation of China[21961160722] ; National Natural Science Foundation of China[91845201] ; International Partnership Program of Chinese Academy of Sciences[172GJHZ2022028MI] ; IMR Innovation Fund[2022-PY05] ; Natural Science Foundation of Liaoning Province[2021-MS-001] ; Guangxi Collaborative Innovation Centre of Structure and Property for New Energy and Materials, Science Research, Technology Development Project of Guilin[20210102-4] ; China Postdoctoral Science Foundation[2021M703279] ; Science and Technology Plan from Liaoning Province[2022-BS-002] ; Innovation Foundation from Institute of Metal Research[2022-PY15]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:001318750400001
出版者AMER CHEMICAL SOC
资助机构National Key R&D Program of China ; National Natural Science Foundation of China ; International Partnership Program of Chinese Academy of Sciences ; IMR Innovation Fund ; Natural Science Foundation of Liaoning Province ; Guangxi Collaborative Innovation Centre of Structure and Property for New Energy and Materials, Science Research, Technology Development Project of Guilin ; China Postdoctoral Science Foundation ; Science and Technology Plan from Liaoning Province ; Innovation Foundation from Institute of Metal Research
源URL  
专题金属研究所_中国科学院金属研究所
通讯作者Wang, Guoqing; Ma, Ding; Liu, Hongyang
作者单位1.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Peoples R China
2.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
4.Chinese Acad Sci, State Key Lab Coal Convers, Inst Coal Chem, Taiyuan 030001, Peoples R China
5.Synfuels China Co Ltd, Natl Energy Ctr Coal Clean Fuel, Beijing 101400, Peoples R China
6.Sichuan Univ, Coll Chem, Natl Engn Lab Ecofriendly Polymer Mat Sichuan, Chengdu 610064, Sichuan, Peoples R China
7.Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, New Cornerstone Sci Lab, Beijing 100871, Peoples R China
8.Hong Kong Univ Sci & Technol, Dept Phys, Kowloon, Hong Kong 999077, Peoples R China
9.Hong Kong Univ Sci & Technol, Ctr Quantum Mat, Kowloon, Hong Kong 999077, Peoples R China
10.Sinopec Beijing Res Inst Chem Ind, Beijing 100013, Peoples R China
推荐引用方式
GB/T 7714		 Sui, Chengquan,Ma, Huan,Huang, Fei,et al. Fully Exposed Nickel Clusters for Semihydrogenation of Acetylene[J]. ACS CATALYSIS,2024,14(19):14689-14695.
APA Sui, Chengquan.,Ma, Huan.,Huang, Fei.,Wang, Maolin.,Cai, Xiangbin.,...&Liu, Hongyang.(2024).Fully Exposed Nickel Clusters for Semihydrogenation of Acetylene.ACS CATALYSIS,14(19),14689-14695.
MLA Sui, Chengquan,et al."Fully Exposed Nickel Clusters for Semihydrogenation of Acetylene".ACS CATALYSIS 14.19(2024):14689-14695.

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来源：金属研究所

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