4.8 Article

Highly Efficient Performance and Conversion Pathway of Photocatalytic NO Oxidation on SrO-Clusters@Amorphous Carbon Nitride

期刊

ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 51, 期 18, 页码 10682-10690

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.est.7b00974

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资金

  1. National Key RD project [2016YFC0204702]
  2. National Natural Science Foundation of China [51478070, 21777011, 21501016]
  3. Innovative Research Team of Chongqing [CXTDG201602014]
  4. Natural Science Foundation of Chongqing [cstc2017jcyjBX0052, cstc2016jcyjA0481]

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This work demonstrates the first molecular-level conversion pathway of NO oxidation over a novel SrO-clusters@amorphous carbon nitride (SCO-ACN) photo catalyst, which is synthesized via copyrolysis of urea and SrCO3. The inclusion of SrCO3 is crucial in the formation of the amorphous carbon nitride (ACN) and SrO clusters by attacking the intralayer hydrogen bonds at the edge sites of graphitic carbon nitride (CN). The amorphous nature of ACN can promote the transportation, migration, and transformation of charge carriers on SCO-ACN. And the SrO clusters are identified as the newly formed active centers to facilitate the activation of NO via the formation of Sr-NO delta(+), which essentially promotes the conversion of NO to the final products. The combined effects of the amorphous structure and SrO clusters impart outstanding photocatalytic NO removal efficiency to the SCO-ACN under visible-light irradiation. To reveal the photocatalytic mechanism, the adsorption and photocatalytic oxidation of NO over CN and SCO-ACN are analyzed by in situ DRIFTS, and the intermediates and conversion pathways are elucidated and compared. This work presents a novel in situ DRIFTS-based strategy to explore the photocatalytic reaction pathway of NO oxidation, which is quite beneficial to understand the mechanism underlying the photocatalytic reaction and advance the development of photocatalytic technology for environmental remediation.

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