4.8 Article

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

Journal

ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 53, Issue 12, Pages 6964-6971

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.est.9b01287

Keywords

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Funding

  1. National Key Research and Development Program of China [2016YFA0203000]
  2. National Natural Science Funds for Distinguished Young Scholars [21425728]
  3. National Natural Science Foundation of China [21477044, 51472100, 21872061]
  4. 111 Project [B17019]
  5. Self-Determined Research Funds of CCNU from the Colleges' Basic Research and Operation of MOE [CCNU16A02029]

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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 (V-O) of BiOCL, a prototypical F center (V-O('')) is a superb site to confine O-2 toward efficient and selective NO oxidation to nitrate. Stimulated by solar light, V-O('') accomplishes NO oxidation through a two-electron charging (V-O('') + O-2 -> V-O('') -O-2(2-)) and subsequent one-electron decharging process (V-O('')-O-2(2)- + NO -> V-O-NO3- + e(-)). The back-donated electron is retrapped by V-O to produce a new single-electron-trapped V-O (V-O(')), simultaneously triggering a second round of NO oxidation (V-O' -O-2 + 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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