Radical Chemistry and Reaction Mechanisms of Propane Oxidative Dehydrogenation over Hexagonal Boron Nitride Catalysts

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

doi:10.1002/anie.202002440

Radical Chemistry and Reaction Mechanisms of Propane Oxidative Dehydrogenation over Hexagonal Boron Nitride Catalysts

Journal Article · Wed Apr 15 00:00:00 EDT 2020 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202002440· OSTI ID:1813272

Zhang, Xuanyu ^[1]; You, Rui ^[2]; Wei, Zeyue ^[2]; ^[1]; Yang, Jiuzhong ^[2]; ^[2]; Wu, Peiwen ^[3]; Jia, Qingdong ^[3]; ^[1]; Bai, Lei ^[1]; ^[4]; ^[1]; ^[1]; ^[2]; ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Science and Technology of China, Hefei (China)
Jiangsu University (China)
Univ. of Tennessee, Knoxville, TN (United States)

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 (CH₃^.) 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 C₂ and C₁ 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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1813272

Alternate ID(s):: OSTI ID: 1615043
OSTI ID: 22937925

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 21 Vol. 59; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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