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Rationalizing kinetic behaviors of isolated boron sites catalyzed oxidative dehydrogenation of propane

Author

Listed:
  • Hao Tian

    (Peking University
    Beijing National Laboratory for Molecular Sciences)

  • Wenying Li

    (Tsinghua University)

  • Linhai He

    (Chinese Academy of Sciences)

  • Yunzhu Zhong

    (Peking University
    Beijing National Laboratory for Molecular Sciences)

  • Shutao Xu

    (Chinese Academy of Sciences)

  • Hai Xiao

    (Tsinghua University)

  • Bingjun Xu

    (Peking University
    Beijing National Laboratory for Molecular Sciences)

Abstract

Boron-based catalysts exhibit high alkene selectivity in oxidative dehydrogenation of propane (ODHP) but the mechanistic understanding remains incomplete. In this work, we show that the hydroxylation of framework boron species via steaming not only enhances the ODHP rate on both B-MFI and B-BEA, but also impacts the kinetics of the reaction. The altered activity, propane reaction order and the activation energy could be attributed to the hydrolysis of framework [B(OSi≡)3] unit to [B(OSi≡)3−x(OH···O(H)Si≡)x] (x = 1, 2, “···” represents hydrogen bonding). DFT calculations confirm that hydroxylated framework boron sites could stabilize radical species, e.g., hydroperoxyl radical, further facilitating the gas-phase radical mechanism. Variations in the contributions from gas-phase radical mechanisms in ODHP lead to the linear correlation between activation enthalpy and entropy on borosilicate zeolites. Insights gained in this work offer a general mechanistic framework to rationalize the kinetic behavior of the ODHP on boron-based catalysts.

Suggested Citation

  • Hao Tian & Wenying Li & Linhai He & Yunzhu Zhong & Shutao Xu & Hai Xiao & Bingjun Xu, 2023. "Rationalizing kinetic behaviors of isolated boron sites catalyzed oxidative dehydrogenation of propane," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42403-2
    DOI: 10.1038/s41467-023-42403-2
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    References listed on IDEAS

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    1. Xiaofeng Gao & Ling Zhu & Feng Yang & Lei Zhang & Wenhao Xu & Xian Zhou & Yongkang Huang & Houhong Song & Lili Lin & Xiaodong Wen & Ding Ma & Siyu Yao, 2023. "Subsurface nickel boosts the low-temperature performance of a boron oxide overlayer in propane oxidative dehydrogenation," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
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