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Title: Photo–thermo Catalytic Oxidation over a TiO2-WO3-Supported Platinum Catalyst

Abstract

Photo–thermo catalysis, which integrates photocatalysis on semiconductors with thermocatalysis on supported nonplasmonic metals, has emerged as an attractive approach to improve catalytic performance. However, an understanding of the mechanisms in operation is missing from both the thermo- and photocatalytic perspectives. Deep insights into photo–thermo catalysis are achieved via the catalytic oxidation of propane (C3H8) over a Pt/TiO2-WO3 catalyst that severely suffers from oxygen poisoning at high O2/C3H8 ratios. After introducing UV/Vis light, the reaction temperature required to achieve 70 % conversion of C3H8 lowers to a record-breaking 90 °C from 324 °C and the apparent activation energy drops from 130 kJ mol-1 to 11 kJ mol-1. Furthermore, the reaction order of O2 is -1.4 in dark but reverses to 0.1 under light, thereby suppressing oxygen poisoning of the Pt catalyst. An underlying mechanism is proposed based on direct evidence of the in-situ-captured reaction intermediates.

Authors:
 [1]; ORCiD logo [1];  [1];  [1];  [2];  [2];  [1];  [3];  [1];  [2]; ORCiD logo [4];  [2]
  1. Chinese Academy of Sciences (CAS), Dalian (China)
  2. Chinese Academy of Sciences (CAS), Dalian (China); Chinese Academy of Sciences (CAS), Beijing (China)
  3. Stony Brook Univ., NY (United States)
  4. Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1637654
Alternate Identifier(s):
OSTI ID: 1631337
Report Number(s):
BNL-216121-2020-JAAM
Journal ID: ISSN 0044-8249;1521-3757
Grant/Contract Number:  
SC0012704; FG02-03ER15476
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie
Additional Journal Information:
Journal Volume: 132; Journal Issue: 31; Journal ID: ISSN 0044-8249
Publisher:
German Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY

Citation Formats

Kang, Leilei, Liu, Xiao Yan, Wang, Aiqin, Li, Lin, Ren, Yujing, Li, Xiaoyu, Pan, Xiaoli, Li, Yuanyuan, Zong, Xu, Liu, Hua, Frenkel, Anatoly I., and Zhang, Tao. Photo–thermo Catalytic Oxidation over a TiO2-WO3-Supported Platinum Catalyst. United States: N. p., 2020. Web. https://doi.org/10.1002/ange.202001701.
Kang, Leilei, Liu, Xiao Yan, Wang, Aiqin, Li, Lin, Ren, Yujing, Li, Xiaoyu, Pan, Xiaoli, Li, Yuanyuan, Zong, Xu, Liu, Hua, Frenkel, Anatoly I., & Zhang, Tao. Photo–thermo Catalytic Oxidation over a TiO2-WO3-Supported Platinum Catalyst. United States. https://doi.org/10.1002/ange.202001701
Kang, Leilei, Liu, Xiao Yan, Wang, Aiqin, Li, Lin, Ren, Yujing, Li, Xiaoyu, Pan, Xiaoli, Li, Yuanyuan, Zong, Xu, Liu, Hua, Frenkel, Anatoly I., and Zhang, Tao. Sun . "Photo–thermo Catalytic Oxidation over a TiO2-WO3-Supported Platinum Catalyst". United States. https://doi.org/10.1002/ange.202001701. https://www.osti.gov/servlets/purl/1637654.
@article{osti_1637654,
title = {Photo–thermo Catalytic Oxidation over a TiO2-WO3-Supported Platinum Catalyst},
author = {Kang, Leilei and Liu, Xiao Yan and Wang, Aiqin and Li, Lin and Ren, Yujing and Li, Xiaoyu and Pan, Xiaoli and Li, Yuanyuan and Zong, Xu and Liu, Hua and Frenkel, Anatoly I. and Zhang, Tao},
abstractNote = {Photo–thermo catalysis, which integrates photocatalysis on semiconductors with thermocatalysis on supported nonplasmonic metals, has emerged as an attractive approach to improve catalytic performance. However, an understanding of the mechanisms in operation is missing from both the thermo- and photocatalytic perspectives. Deep insights into photo–thermo catalysis are achieved via the catalytic oxidation of propane (C3H8) over a Pt/TiO2-WO3 catalyst that severely suffers from oxygen poisoning at high O2/C3H8 ratios. After introducing UV/Vis light, the reaction temperature required to achieve 70 % conversion of C3H8 lowers to a record-breaking 90 °C from 324 °C and the apparent activation energy drops from 130 kJ mol-1 to 11 kJ mol-1. Furthermore, the reaction order of O2 is -1.4 in dark but reverses to 0.1 under light, thereby suppressing oxygen poisoning of the Pt catalyst. An underlying mechanism is proposed based on direct evidence of the in-situ-captured reaction intermediates.},
doi = {10.1002/ange.202001701},
journal = {Angewandte Chemie},
number = 31,
volume = 132,
place = {United States},
year = {2020},
month = {4}
}

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