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Co-infiltration and dynamic formation of Pd3ZnCx intermetallic carbide by syngas boosting selective hydrogenation of acetylene

Author

Listed:
  • Huan Chen

    (Dalian University of Technology
    Chinese Academy of Sciences)

  • Lulu Li

    (Tianjin University)

  • Zhi-Jian Zhao

    (Tianjin University)

  • Bing Yang

    (Chinese Academy of Sciences)

  • Yafeng Zhang

    (Chinese Academy of Sciences)

  • Xiaoyan Liu

    (Chinese Academy of Sciences)

  • Qingqing Gu

    (Chinese Academy of Sciences)

  • Zhounan Yu

    (Chinese Academy of Sciences)

  • Xiaofeng Yang

    (Chinese Academy of Sciences)

  • Jinlong Gong

    (Tianjin University
    Tianjin Normal University)

  • Aiqin Wang

    (Chinese Academy of Sciences)

  • Tao Zhang

    (Dalian University of Technology
    Chinese Academy of Sciences)

Abstract

Transition metal carbide shows excellent performance in selective hydrogenation of acetylene, however, the carburization of Pd-based intermetallic compounds remains infeasible. Here we report the successful synthesis of an unprecedented Pd3ZnCx intermetallic carbide, via co-infiltration of zinc and carbon in one-step carburization by syngas. Utilizing state-of-the-art in situ characterizations and theoretical calculation, we unveil the dynamic evolution of Pd3ZnCx during carburization, forming a Pd3Zn like cubic phase carbide structure. A unique transitional state (Pdt) with low content of Zn/C co-infiltration is clearly identified facilitating phase transition and sustain incorporation of carbon and zinc at elevated temperatures. The Pd3ZnCx carbide shows by far the best catalytic performance in the selective hydrogenation of acetylene with a high selectivity (>90%) even at a high H2/C2H2 ratio. Our results therefore provide a co-infiltration strategy and dynamic insights for the one-step synthesis of Pd based intermetallic carbides, towards high-performance intermetallic compound for selective hydrogenation of acetylene.

Suggested Citation

  • Huan Chen & Lulu Li & Zhi-Jian Zhao & Bing Yang & Yafeng Zhang & Xiaoyan Liu & Qingqing Gu & Zhounan Yu & Xiaofeng Yang & Jinlong Gong & Aiqin Wang & Tao Zhang, 2024. "Co-infiltration and dynamic formation of Pd3ZnCx intermetallic carbide by syngas boosting selective hydrogenation of acetylene," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-54274-2
    DOI: 10.1038/s41467-024-54274-2
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    References listed on IDEAS

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    1. Yiming Niu & Xing Huang & Yongzhao Wang & Ming Xu & Junnan Chen & Shuliang Xu & Marc-Georg Willinger & Wei Zhang & Min Wei & Bingsen Zhang, 2020. "Manipulating interstitial carbon atoms in the nickel octahedral site for highly efficient hydrogenation of alkyne," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    2. Mengyao Ouyang & Konstantinos G. Papanikolaou & Alexey Boubnov & Adam S. Hoffman & Georgios Giannakakis & Simon R. Bare & Michail Stamatakis & Maria Flytzani-Stephanopoulos & E. Charles H. Sykes, 2021. "Directing reaction pathways via in situ control of active site geometries in PdAu single-atom alloy catalysts," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
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