Interfacial Charging–Decharging Strategy for Efficient and Selective Aerobic NO Oxidation on Oxygen Vacancy

  • Hao Li
    Hao Li
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Applied & Environmental Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
    More by Hao Li
  • Huan Shang
    Huan Shang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Applied & Environmental Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
    More by Huan Shang
  • Yuhan Li
    Yuhan Li
    Chongqing Key Laboratory of Catalysis and New Environmental Materials, Engineering Research Center for Waste Oil Recovery Technology and Equipment, Ministry of Education, College of Environment and Resources, Chongqing Technology and Business University, Chongqing 400067, China
    More by Yuhan Li
  • Xuemei Cao
    Xuemei Cao
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Applied & Environmental Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
    More by Xuemei Cao
  • Zhiping Yang
    Zhiping Yang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Applied & Environmental Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
    More by Zhiping Yang
  • Zhihui Ai*
    Zhihui Ai
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Applied & Environmental Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
    *(Z.A.) Phone/Fax: +86-27-6786 7535; e-mail: [email protected]
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  • , and 
  • Lizhi Zhang*
    Lizhi Zhang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Applied & Environmental Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
    *(L.Z.) E-mail: [email protected]
    More by Lizhi Zhang
Cite this: Environ. Sci. Technol. 2019, 53, 12, 6964–6971
Publication Date (Web):May 14, 2019
https://doi.org/10.1021/acs.est.9b01287
Copyright © 2019 American Chemical Society
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Abstract

Intelligent defect engineering to harness surface molecular processes is at the core of selective oxidation catalysis. Here, we demonstrate that the two-electron-trapped oxygen vacancy (VO) of BiOCl, a prototypical F center (VŐ′′), is a superb site to confine O2 toward efficient and selective NO oxidation to nitrate. Stimulated by solar light, VŐ′′ accomplishes NO oxidation through a two-electron charging (VŐ′′ + O2 → VŐ′′-O22–) and subsequent one-electron decharging process (VŐ′′-O22– + NO → VO-NO3 + e). The back-donated electron is retrapped by VO to produce a new single-electron-trapped VO (VO′), simultaneously triggering a second round of NO oxidation (VO′-O2 + NO → VO-NO3). This unprecedented interfacial charging–decharging scheme alters the peroxide-associated NO oxidation selectivity from NO2 to NO3 with a high efficiency and thus hold great promise for the treatment of risky NOx species in indoor air.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.9b01287.

  • Theoretical results of •O2-associated NO oxidation; morphology and phase structure of the as-prepared BiOCl photocatalysts; XPS spectra and PL spectra; designed reaction cell for the in situ IR signal recording; quantitative determination of •O2 and O22-; photocatalytic NO removal over BiOCl with different concentrations of VO; desorption energy diagram of nitrate from BiOCl; influence of catalase and tert-butyl alcohol on the photocatalytic NO removal; recycled NO removal; parameters of the time-resolved photoluminescence decay curves (PDF)

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