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

被引:126
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
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