Volume 8 Issue 4
Aug.  2023
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Article Navigation >  Green Energy&Environment  > 2023  >  8(4): 1141-1153
Yang Yang, Chaoyue Zhao, Xianliang Qiao, Qingxin Guan, Wei Li. Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorination. Green Energy&Environment, 2023, 8(4): 1141-1153. doi: 10.1016/j.gee.2022.01.006
Citation: Yang Yang, Chaoyue Zhao, Xianliang Qiao, Qingxin Guan, Wei Li. Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorination. Green Energy&Environment, 2023, 8(4): 1141-1153. doi: 10.1016/j.gee.2022.01.006
shu

Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorination

doi: 10.1016/j.gee.2022.01.006

  • State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, No. 94 Weijin Road, Tianjin, 300071, China

Funds:

This work was supported by the National Natural Science Foundation of China (NSFC, 22172082, 21978137, 22102074, and 21878162), Natural Science Foundation of Tianjin (20JCZDJC00770), Postdoctoral Research Foundation of China (2021M701776), NCC Fund (NCC2020FH05), and dedicated to the 100th anniversary of Chemistry at Nankai University.

  • Received date 21 October 2021, Accepted date 12 January 2022, RevRecd date 21 December 2021, Available online 07 July 2023, Publish date 20 January 2022,
    Abstract
  • In this work, DFT calculations were used firstly to simulate the nitrogen coordinated metal single-atom catalysts (M-Nx SACs, M = Hg, Cu, Au, and Ru) to predict their catalytic activities in acetylene hydrochlorination. The DFT results showed that Ru-Nx SACs had the best catalytic performance among the four catalysts, and Ru-Nx SACs could effectively inhibit the reduction of ruthenium cation. To verify the DFT results, Ru-Nx SACs were fabricated by pyrolyzing MOFs in-situ spatially confined metal precursors. The N coordination environment could be controlled by changing the pyrolysis temperature. Catalytic performance tests indicated that low N coordination number (Ru–N2, Ru–N3) exhibited excellent catalytic activity and stability compared to RuCl3 catalyst. DFT calculations further revealed that Ru–N2 and Ru–N3 had a tendency to activate HCl at the first step of reaction, whereas Ru–N4 tended to activate C2H2. These findings will serve as a reference for the design and control of metal active sites.

     

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