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

Hao Tian, Wenying Li, Linhai He, Yunzhu Zhong, Shutao Xu, Hai Xiao and Bingjun Xu ()
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Hao Tian: Peking University
Wenying Li: Tsinghua University
Linhai He: Chinese Academy of Sciences
Yunzhu Zhong: Peking University
Shutao Xu: Chinese Academy of Sciences
Hai Xiao: Tsinghua University
Bingjun Xu: Peking University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-42403-2

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