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Structure-dependence and metal-dependence on atomically dispersed Ir catalysts for efficient n-butane dehydrogenation

Author

Listed:
  • Xiaowen Chen

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Xuetao Qin

    (College of Chemistry and Molecular Engineering, Peking University)

  • Yueyue Jiao

    (Chinese Academy of Sciences
    Synfuels China Co., Ltd
    The University of Chinese Academy of Sciences)

  • Mi Peng

    (College of Chemistry and Molecular Engineering, Peking University)

  • Jiangyong Diao

    (Chinese Academy of Sciences)

  • Pengju Ren

    (Chinese Academy of Sciences
    Synfuels China Co., Ltd)

  • Chengyu Li

    (College of Chemistry and Molecular Engineering, Peking University)

  • Dequan Xiao

    (University of New Haven)

  • Xiaodong Wen

    (Chinese Academy of Sciences
    Synfuels China Co., Ltd)

  • Zheng Jiang

    (Chinese Academy of Sciences)

  • Ning Wang

    (Hong Kong University of Science and Technology)

  • Xiangbin Cai

    (Hong Kong University of Science and Technology)

  • Hongyang Liu

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Ding Ma

    (College of Chemistry and Molecular Engineering, Peking University)

Abstract

Single-site pincer-ligated iridium complexes exhibit the ability for C-H activation in homogeneous catalysis. However, instability and difficulty in catalyst recycling are inherent disadvantages of the homogeneous catalyst, limiting its development. Here, we report an atomically dispersed Ir catalyst as the bridge between homogeneous and heterogeneous catalysis, which displays an outstanding catalytic performance for n-butane dehydrogenation, with a remarkable n-butane reaction rate (8.8 mol·gIr−1·h−1) and high butene selectivity (95.6%) at low temperature (450 °C). Significantly, we correlate the BDH activity with the Ir species from nanoscale to sub-nanoscale, to reveal the nature of structure-dependence of catalyst. Moreover, we compare Ir single atoms with Pt single atoms and Pd single atoms for in-depth understanding the nature of metal-dependence at the atomic level. From experimental and theoretical calculations results, the isolated Ir site is suitable for both reactant adsorption/activation and product desorption. Its remarkable dehydrogenation capacity and moderate adsorption behavior are the key to the outstanding catalytic activity and selectivity.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-38361-4
    DOI: 10.1038/s41467-023-38361-4
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    References listed on IDEAS

    as
    1. Zhibo Liu & Fei Huang & Mi Peng & Yunlei Chen & Xiangbin Cai & Linlin Wang & Zenan Hu & Xiaodong Wen & Ning Wang & Dequan Xiao & Hong Jiang & Hongbin Sun & Hongyang Liu & Ding Ma, 2021. "Tuning the selectivity of catalytic nitriles hydrogenation by structure regulation in atomically dispersed Pd catalysts," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    2. Guodong Sun & Zhi-Jian Zhao & Rentao Mu & Shenjun Zha & Lulu Li & Sai Chen & Ketao Zang & Jun Luo & Zhenglong Li & Stephen C. Purdy & A. Jeremy Kropf & Jeffrey T. Miller & Liang Zeng & Jinlong Gong, 2018. "Breaking the scaling relationship via thermally stable Pt/Cu single atom alloys for catalytic dehydrogenation," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    3. Zijun Huang & Dedong He & Weihua Deng & Guowu Jin & Ke Li & Yongming Luo, 2023. "Illustrating new understanding of adsorbed water on silica for inducing tetrahedral cobalt(II) for propane dehydrogenation," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    4. 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.
    5. 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. "Author Correction: Regulating coordination number in atomically dispersed Pt species on defect-rich graphene for n-2 butane dehydrogenation reaction," Nature Communications, Nature, vol. 12(1), pages 1-1, December.
    6. Qilun Wang & Cong-Qiao Xu & Wei Liu & Sung-Fu Hung & Hong Yang & Jiajian Gao & Weizheng Cai & Hao Ming Chen & Jun Li & Bin Liu, 2020. "Coordination engineering of iridium nanocluster bifunctional electrocatalyst for highly efficient and pH-universal overall water splitting," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
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