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Radical Chemistry and Reaction Mechanisms of Propane Oxidative Dehydrogenation over Hexagonal Boron Nitride Catalysts
Author(s) -
Zhang Xuanyu,
You Rui,
Wei Zeyue,
Jiang Xiao,
Yang Jiuzhong,
Pan Yang,
Wu Peiwen,
Jia Qingdong,
Bao Zhenghong,
Bai Lei,
Jin Mingzhou,
Sumpter Bobby,
Fung Victor,
Huang Weixin,
Wu Zili
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202002440
Subject(s) - dehydrogenation , catalysis , propene , chemistry , propane , boron , photochemistry , density functional theory , boron nitride , radical , reaction mechanism , inorganic chemistry , computational chemistry , organic chemistry
Although hexagonal boron nitride (h‐BN) has recently been identified as a highly efficient catalyst for the oxidative dehydrogenation of propane (ODHP) reaction, the reaction mechanisms, especially regarding radical chemistry of this system, remain elusive. Now, the first direct experimental evidence of gas‐phase methyl radicals (CH 3 . ) in the ODHP reaction over boron‐based catalysts is achieved by using online synchrotron vacuum ultraviolet photoionization mass spectroscopy (SVUV‐PIMS), which uncovers the existence of gas‐phase radical pathways. Combined with density functional theory (DFT) calculations, the results demonstrate that propene is mainly generated on the catalyst surface from the C−H activation of propane, while C 2 and C 1 products can be formed via both surface‐mediated and gas‐phase pathways. These observations provide new insights towards understanding the ODHP reaction mechanisms over boron‐based catalysts.