Oxygen Vacancies Promoted the Selective Photocatalytic Removal of NO with Blue TiO2 via Simultaneous Molecular Oxygen Activation and Photogenerated Hole Annihilation

  • Huan Shang
    Huan Shang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Huan Shang
  • Meiqi Li
    Meiqi Li
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Meiqi Li
  • Hao Li
    Hao Li
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Hao Li
  • Shun Huang
    Shun Huang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    More by Shun Huang
  • Chengliang Mao
    Chengliang Mao
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
  • Zhihui Ai*
    Zhihui Ai
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    *Phone/fax: +86-27-6786 7535; e-mail: [email protected]
    More by Zhihui Ai
  • , and 
  • Lizhi Zhang*
    Lizhi Zhang
    Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
    *E-mail: [email protected]
    More by Lizhi Zhang
Cite this: Environ. Sci. Technol. 2019, 53, 11, 6444–6453
Publication Date (Web):May 3, 2019
Copyright © 2019 American Chemical Society
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Semiconductor photocatalytic technology has great potential for the removal of dilute gaseous NO in indoor and outdoor atmospheres but suffers from unsatisfactory NO-removal selectivity due to undesirable NO2 byproduct generation. In this study, we demonstrate that the 99% selectivity of photocatalytic NO oxidation toward nitrate can be achieved over blue TiO2 bearing oxygen vacancies (OVs) under visible-light irradiation. First-principles density functional theory calculation and experimental results suggested that the OVs of blue TiO2 with localized electrons could facilitate the molecular oxygen activation through single-electron pathways to generate ·O2 and simultaneously promote the photogenerated hole annihilation. The generated ·O2 directly converted NO to nitrate, while the hole annihilation inhibited the side-reaction between holes and NO to avoid toxic NO2 byproduct formation, resulting in the highly selective removal of NO. This study reveals the dual functions of OVs in defective photocatalysts and also provides fundamental guidance for the selective purification of NO with photocatalytic technology.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.8b07322.

  • Figures showing Surface coordination structures, NO and O2 adsorption on TiO2 and TiO2-OV surface, TEM images and XPS spectra, photographs of the as-prepared TiO2-OV and TiO2, BET characterization and first-order kinetic constants calculation, the selectivity of NO, ionic chromatography, product distributions, capture experiments, FTIR spectra, photocatalytic NO2 oxidation, the influence of OVs on photocatalytic NO oxidation, solid EPR measurement, electrochemical characterization, EPR measurement, 1H NMR spectra, and the influence of surface hydrogen on photocatalytic NO oxidation; tables showing calculated absorption energy and Bader charges and parameters of the time-resolved photoluminescence decay curves. (PDF)

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