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Oxygen Vacancy Promoted O2 Activation over Perovskite Oxide for Low-Temperature CO Oxidation

  • Ji Yang
    Ji Yang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Ji Yang
  • Siyu Hu
    Siyu Hu
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Siyu Hu
  • Yarong Fang
    Yarong Fang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Yarong Fang
  • Son Hoang
    Son Hoang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Son Hoang
  • Li Li
    Li Li
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Li Li
  • Weiwei Yang
    Weiwei Yang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Weiwei Yang
  • Zhenfeng Liang
    Zhenfeng Liang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
  • Jian Wu
    Jian Wu
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Jian Wu
  • Jinpeng Hu
    Jinpeng Hu
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Jinpeng Hu
  • Wen Xiao
    Wen Xiao
    Department of Materials Science and Engineering, National University of Singapore, Singapore 117576, Singapore
    More by Wen Xiao
  • Chuanqi Pan
    Chuanqi Pan
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Chuanqi Pan
  • Zhu Luo
    Zhu Luo
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Zhu Luo
  • Jun Ding
    Jun Ding
    Department of Materials Science and Engineering, National University of Singapore, Singapore 117576, Singapore
    More by Jun Ding
  • Lizhi Zhang
    Lizhi Zhang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Lizhi Zhang
  • , and 
  • Yanbing Guo*
    Yanbing Guo
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    *E-mail: [email protected]. Phone: +86-17786507005.
    More by Yanbing Guo
Cite this: ACS Catal. 2019, 9, 11, 9751–9763
Publication Date (Web):September 18, 2019
https://doi.org/10.1021/acscatal.9b02408
Copyright © 2019 American Chemical Society
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Abstract

The insights on the primary active oxygen specie and its relation with oxygen vacancy is essential for the design of low-temperature oxidation catalysts. Herein, oxygen vacancy-rich La0.8Sr0.2CoO3 with an ordered macroporous structure was integrated on the commercial ceramic monolith in large scale without additional adhesives via a facile in situ solution assembly. The constructed macropores not only contributed to the oxygen vacancy generation in catalyst preparation but also facilitated favorable mass transport during catalytic process. Combined with theoretical investigations and EPR, O2-TPD, H2-TPR observations, we revealed that monatomic oxygen ions (O) are the primary oxygen active specie for perovskite oxide. And molecular O2 is more favorably adsorbed and activated on surface oxygen vacancies via a one electron transfer process to form monatomic oxygen ions (O), thus boosting richness of active O and the low-temperature oxidation of CO. Different with the preferential Eley–Rideal (E-R) mechanism on pristine LSCO surface, Langmuir–Hinshelwood (L-H) mechanism, in which O reacts with adsorbed CO to finish the oxidation reaction, was more favorable on the oxygen vacancy rich surface. Our work here elucidates the primary active oxygen specie as well as its origin over perovskite oxides and paves a feasible pathway for rational design of high-performance catalysts in heterogeneous reactions.

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