Regulating coordination number in atomically dispersed Pt species on defect-rich graphene for n-butane dehydrogenation reaction

Xiaowen Chen, Mi Peng, Xiangbin Cai, Yunlei Chen, Zhimin Jia, Yuchen Deng, Bingbao Mei, Zheng Jiang, Dequan Xiao, Xiaodong Wen, Ning Wang (), Hongyang Liu () and Ding Ma ()
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Xiaowen Chen: Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences
Mi Peng: Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering and College of Engineering, and BIC-ESAT, Peking University
Xiangbin Cai: Department of Physics and Center for Quantum Materials, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon
Yunlei Chen: State Key Laboratory of Coal Conversion, Institute Coal Chemistry, Chinese Academy of Sciences
Zhimin Jia: Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences
Yuchen Deng: Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering and College of Engineering, and BIC-ESAT, Peking University
Bingbao Mei: Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Zheng Jiang: Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Dequan Xiao: Center for Integrative Materials Discovery, Department of Chemistry and Chemical Engineering, University of New Haven
Xiaodong Wen: State Key Laboratory of Coal Conversion, Institute Coal Chemistry, Chinese Academy of Sciences
Ning Wang: Department of Physics and Center for Quantum Materials, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon
Hongyang Liu: Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences
Ding Ma: Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering and College of Engineering, and BIC-ESAT, Peking University

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Metal nanoparticle (NP), cluster and isolated metal atom (or single atom, SA) exhibit different catalytic performance in heterogeneous catalysis originating from their distinct nanostructures. To maximize atom efficiency and boost activity for catalysis, the construction of structure–performance relationship provides an effective way at the atomic level. Here, we successfully fabricate fully exposed Pt3 clusters on the defective nanodiamond@graphene (ND@G) by the assistance of atomically dispersed Sn promoters, and correlated the n-butane direct dehydrogenation (DDH) activity with the average coordination number (CN) of Pt-Pt bond in Pt NP, Pt3 cluster and Pt SA for fundamentally understanding structure (especially the sub-nano structure) effects on n-butane DDH reaction at the atomic level. The as-prepared fully exposed Pt3 cluster catalyst shows higher conversion (35.4%) and remarkable alkene selectivity (99.0%) for n-butane direct DDH reaction at 450 °C, compared to typical Pt NP and Pt SA catalysts supported on ND@G. Density functional theory calculation (DFT) reveal that the fully exposed Pt3 clusters possess favorable dehydrogenation activation barrier of n-butane and reasonable desorption barrier of butene in the DDH reaction.

Date: 2021
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DOI: 10.1038/s41467-021-22948-w

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