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

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  • Xiaowen Chen

    (Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences
    School of Materials Science and Engineering, University of Science and Technology of China)

  • 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
    University of Chinese Academy of Science)

  • Zhimin Jia

    (Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences
    School of Materials Science and Engineering, University of Science and Technology of China)

  • 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
    University of Chinese Academy of Science)

  • 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
    School of Materials Science and Engineering, University of Science and Technology of China)

  • Ding Ma

    (Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering and College of Engineering, and BIC-ESAT, Peking University)

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.

Suggested Citation

  • Xiaowen Chen & Mi Peng & Xiangbin Cai & Yunlei Chen & Zhimin Jia & Yuchen Deng & Bingbao Mei & Zheng Jiang & Dequan Xiao & Xiaodong Wen & Ning Wang & Hongyang Liu & Ding Ma, 2021. "Regulating coordination number in atomically dispersed Pt species on defect-rich graphene for n-butane dehydrogenation reaction," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-22948-w
    DOI: 10.1038/s41467-021-22948-w
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    Cited by:

    1. Zhirong Zhang & Chen Feng & Dongdi Wang & Shiming Zhou & Ruyang Wang & Sunpei Hu & Hongliang Li & Ming Zuo & Yuan Kong & Jun Bao & Jie Zeng, 2022. "Selectively anchoring single atoms on specific sites of supports for improved oxygen evolution," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Xin Zhao & Fengliang Wang & Xiangpeng Kong & Ruiqi Fang & Yingwei Li, 2022. "Subnanometric Cu clusters on atomically Fe-doped MoO2 for furfural upgrading to aviation biofuels," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    3. Jiaqi Zhao & Jinjia Liu & Zhenhua Li & Kaiwen Wang & Run Shi & Pu Wang & Qing Wang & Geoffrey I. N. Waterhouse & Xiaodong Wen & Tierui Zhang, 2023. "Ruthenium-cobalt single atom alloy for CO photo-hydrogenation to liquid fuels at ambient pressures," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    4. Xiaowen Chen & Xuetao Qin & Yueyue Jiao & Mi Peng & Jiangyong Diao & Pengju Ren & Chengyu Li & Dequan Xiao & Xiaodong Wen & Zheng Jiang & Ning Wang & Xiangbin Cai & Hongyang Liu & Ding Ma, 2023. "Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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