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作者:

Hailili, Reshalaiti (Hailili, Reshalaiti.) | Ji, Hongwei (Ji, Hongwei.) | Wang, Kaiwen (Wang, Kaiwen.) | Dong, Xing'an (Dong, Xing'an.) | Chen, Chuncheng (Chen, Chuncheng.) | Sheng, Hua (Sheng, Hua.) | Bahnemann, Detlef W. (Bahnemann, Detlef W..) | Zhao, Jincai (Zhao, Jincai.)

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EI Scopus SCIE

摘要:

Semiconductor-based photocatalysis is an ideal method for air purification by eliminating nitrogen oxide (NO). However, sluggish carrier separation, photocatalysts deactivation and incomplete oxidation are significant bottlenecks for photocatalytic treatment of indoor pollutant NO. Herein, ZnO with assorted structures is fabricated and undergoes further modification for deliberate surface defect constructions. Utilized flux agents during the synthesis provide a more feasible reducing atmosphere, under which spontaneous generations of the surface vacancies become easier, and gradient concentrations are precisely controlled. Photocatalyst characterizations affirm the successful creation of surface defects, which are further evaluated by solar-light-driven NO (ppb level) removal investigations. Results showed that ZnO rich in oxygen vacancies (V-O-rich ZnO) exhibited 5.43 and 1.63 times enhanced NO removal with fewer toxic product NO2 formations than its counterparts pristine and Vo-poor ZnO, respectively. Importantly, with higher V-O on the unusual nonpolar facets, V-O-rich ZnO does not only display enhanced NO conversion, but also shows the unselective NO removal process by producing NO3-. The plausible reaction mechanisms of promoted NO conversions are further investigated based on the surface V-O, well-positioned band structures, and enhanced carrier separations. Results showed that the surface V-O with gradient concentrations are not only promoted carrier separation, but also facilitate molecular oxygen activation, leading to the generations of strong oxidant superoxide radicals (center dot O-2(-)), and contributing to the enhanced improved efficiency. Adsorption of small molecules (O-2, H2O and NO) on the defective surface was further investigated by density functional theory (DFT) calculations, which validated the successful adsorption/activation of NO and O-2, further contributed to the improved NO conversions.

关键词:

carrier separation photocatalysis surface-interface surface defects NO removal

作者机构:

  • [ 1 ] [Hailili, Reshalaiti]Chinese Acad Sci, Inst Chem, Key Lab Photochem, Beijing 100190, Peoples R China
  • [ 2 ] [Ji, Hongwei]Chinese Acad Sci, Inst Chem, Key Lab Photochem, Beijing 100190, Peoples R China
  • [ 3 ] [Dong, Xing'an]Chinese Acad Sci, Inst Chem, Key Lab Photochem, Beijing 100190, Peoples R China
  • [ 4 ] [Chen, Chuncheng]Chinese Acad Sci, Inst Chem, Key Lab Photochem, Beijing 100190, Peoples R China
  • [ 5 ] [Sheng, Hua]Chinese Acad Sci, Inst Chem, Key Lab Photochem, Beijing 100190, Peoples R China
  • [ 6 ] [Zhao, Jincai]Chinese Acad Sci, Inst Chem, Key Lab Photochem, Beijing 100190, Peoples R China
  • [ 7 ] [Hailili, Reshalaiti]Leibniz Univ Hannover, Inst Tech Chem, D-30167 Hannover, Germany
  • [ 8 ] [Bahnemann, Detlef W.]Leibniz Univ Hannover, Inst Tech Chem, D-30167 Hannover, Germany
  • [ 9 ] [Hailili, Reshalaiti]Beijing Univ Technol, MOE Key Lab Enhanced Heat Transfer & Energy Conse, Beijing Key Lab Heat Transfer & Energy Convers, Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China
  • [ 10 ] [Wang, Kaiwen]Beijing Univ Technol, MOE Key Lab Enhanced Heat Transfer & Energy Conse, Beijing Key Lab Heat Transfer & Energy Convers, Key Lab Microstruct & Properties Adv Mat, Beijing 100124, Peoples R China

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来源 :

ACS CATALYSIS

ISSN: 2155-5435

年份: 2022

期: 16

卷: 12

页码: 10004-10017

1 2 . 9

JCR@2022

1 2 . 9 0 0

JCR@2022

ESI学科: CHEMISTRY;

ESI高被引阀值:53

JCR分区:1

中科院分区:1

被引次数:

WoS核心集被引频次: 86

SCOPUS被引频次:

ESI高被引论文在榜: 0 展开所有

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