Low-Temperature Acetylene Semi-Hydrogenation over the Pd1-Cu1 Dual-Atom Catalyst

被引:154
作者
Huang, Fei [1 ]
Peng, Mi [2 ]
Chen, Yunlei [3 ]
Cai, Xiangbin [4 ,5 ]
Qin, Xuetao [2 ]
Wang, Ning [4 ,5 ]
Xiao, Dequan [6 ]
Jin, Li [7 ]
Wang, Guoqing [7 ]
Wen, Xiao-Dong [3 ]
Liu, Hongyang [1 ]
Ma, Ding [2 ]
机构
[1] Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
[2] Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Engn, Beijing 100871, Peoples R China
[3] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
[4] Hong Kong Univ Sci & Technol, Dept Phys, Kowloon, Hong Kong 999077, Peoples R China
[5] Hong Kong Univ Sci & Technol, Ctr Quantum Mat, Kowloon, Hong Kong 999077, Peoples R China
[6] Univ New Haven, Ctr Integrat Mat Discovery, Dept Chem & Chem Engn, West Haven, CT 06516 USA
[7] SINOPEC Beijing Res Inst Chem Ind Co Ltd, Beijing 100013, Peoples R China
基金
国家重点研发计划; 中国博士后科学基金;
关键词
SELECTIVE HYDROGENATION; SITES;
D O I
10.1021/jacs.2c07208
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The atomically dispersed metal catalyst or single-atom catalyst (SAC) with the utmost metal utilization efficiency shows excellent selectivity toward ethylene compared to the metal nanoparticles catalyst in the acetylene semi-hydrogenation reaction. However, these catalysts normally work at relatively high temperatures. Achieving low-temperature reactivity while preserv-ing high selectivity remains a challenge. To improve the intrinsic reactivity of SACs, rationally tailoring the coordination environ-ments of the first metal atom by coordinating it with a second neighboring metal atom affords an opportunity. Here, we report the fabrication of a dual-atom catalyst (DAC) that features a bonded Pd1-Cu1 atomic pair anchoring on nanodiamond graphene (ND@ G). Compared to the single-atom Pd or Cu catalyst, it exhibits increased reactivity at a lower temperature, with 100% acetylene conversion and 92% ethylene selectivity at 110 degrees C. This work provides a strategy for designing DACs for low-temperature hydrogenation by manipulating the coordination environment of catalytic sites at the atomic level.
引用
收藏
页码:18485 / 18493
页数:9
相关论文
共 35 条
[1]   Highly Active and Stable Single-Atom Cu Catalysts Supported by a Metal-Organic Framework [J].
Abdel-Mageed, Ali M. ;
Rungtaweevoranit, Bunyarat ;
Parlinska-Wojtan, Magdalena ;
Pei, Xiaokun ;
Yaghi, Omar M. ;
Behm, R. Juergen .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2019, 141 (13) :5201-5210
[2]   Interstitial modification of palladium nanoparticles with boron atoms as a green catalyst for selective hydrogenation [J].
Chan, Chun Wong Aaron ;
Mahadi, Abdul Hanif ;
Li, Molly Meng-Jung ;
Corbos, Elena Cristina ;
Tang, Chiu ;
Jones, Glenn ;
Kuo, Winson Chun Hsin ;
Cookson, James ;
Brown, Christopher Michael ;
Bishop, Peter Trenton ;
Tsang, Shik Chi Edman .
NATURE COMMUNICATIONS, 2014, 5
[3]   Atomically Dispersed Copper-Platinum Dual Sites Alloyed with Palladium Nanorings Catalyze the Hydrogen Evolution Reaction [J].
Chao, Tingting ;
Luo, Xuan ;
Chen, Wenxing ;
Jiang, Bin ;
Ge, Jingjie ;
Lin, Yue ;
Wu, Geng ;
Wang, Xiaoqian ;
Hu, Yanmin ;
Zhuang, Zhongbin ;
Wu, Yuen ;
Hong, Xun ;
Li, Yadong .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (50) :16047-16051
[4]   Few-Atom Pt Ensembles Enable Efficient Catalytic Cyclohexane Dehydrogenation for Hydrogen Production [J].
Deng, Yuchen ;
Guo, Yu ;
Jia, Zhimin ;
Liu, Jin-Cheng ;
Guo, Jinqiu ;
Cai, Xiangbin ;
Dong, Chunyang ;
Wang, Meng ;
Li, Chengyu ;
Diao, Jiangyong ;
Jiang, Zheng ;
Xie, Jinglin ;
Wang, Ning ;
Xiao, Hai ;
Xu, Bingjun ;
Zhang, Hongbo ;
Liu, Hongyang ;
Li, Jun ;
Ma, Ding .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2022, 144 (08) :3535-3542
[5]   Activating Edge Sites on Pd Catalysts for Selective Hydrogenation of Acetylene via Selective Ga2O3 Decoration [J].
Ding, Liangbing ;
Yi, Hong ;
Zhang, Wenhua ;
You, Rui ;
Cao, Tian ;
Yang, Jinlong ;
Lu, Junling ;
Huang, Weixin .
ACS CATALYSIS, 2016, 6 (06) :3700-3707
[6]   Fully exposed palladium cluster catalysts enable hydrogen production from nitrogen heterocycles [J].
Dong, Chunyang ;
Gao, Zirui ;
Li, Yinlong ;
Peng, Mi ;
Wang, Meng ;
Xu, Yao ;
Li, Chengyu ;
Xu, Ming ;
Deng, Yuchen ;
Qin, Xuetao ;
Huang, Fei ;
Wei, Xuyan ;
Wang, Yang-Gang ;
Liu, Hongyang ;
Zhou, Wu ;
Ma, Ding .
NATURE CATALYSIS, 2022, 5 (06) :485-493
[7]   Isolated Single-Atom Pd Sites in Intermetallic Nanostructures: High Catalytic Selectivity for Semihydrogenation of Alkynes [J].
Feng, Quanchen ;
Zhao, Shu ;
Wang, Yu ;
Dong, Juncai ;
Chen, Wenxing ;
He, Dongsheng ;
Wang, Dingshen ;
Yang, Jun ;
Zhu, Yuanmin ;
Zhu, Hailiang ;
Gu, Lin ;
Li, Zhi ;
Liu, Yuxi ;
Yu, Rong ;
Li, Jun ;
Li, Yadong .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (21) :7294-7301
[8]   Electronic structure and catalysis on metal surfaces [J].
Greeley, J ;
Norskov, JK ;
Mavrikakis, M .
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, 2002, 53 :319-348
[9]  
Hammer B, 2000, ADV CATAL, V45, P71
[10]   Atomic Structure and Dynamics of Metal Dopant Pairs in Graphene [J].
He, Zhengyu ;
He, Kuang ;
Robertson, Alex W. ;
Kirkland, Angus I. ;
Kim, Dongwook ;
Ihm, Jisoon ;
Yoon, Euijoon ;
Lee, Gun-Do ;
Warner, Jamie H. .
NANO LETTERS, 2014, 14 (07) :3766-3772