Unraveling the mechanisms of S-doped carbon nitride for photocatalytic oxygen reduction to H2O2
| Autor: | Wei Lin, Yongfan Zhang, Changgeng Wei, Yi Li, Yawen Tong |
|---|---|
| Rok vydání: | 2020 |
| Předmět: |
Reaction mechanism
Materials science Band gap General Physics and Astronomy Charge density 02 engineering and technology Nitride 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences 0104 chemical sciences Catalysis chemistry.chemical_compound chemistry Chemical engineering Photocatalysis Redistribution (chemistry) Physical and Theoretical Chemistry 0210 nano-technology Carbon nitride |
| Zdroj: | Physical Chemistry Chemical Physics. 22:21099-21107 |
| ISSN: | 1463-9084 1463-9076 |
| DOI: | 10.1039/d0cp03533e |
| Popis: | An in-depth understanding of the microscopic reaction mechanism on a nonmetal-doped catalytic system at the atomic level is one of the critical approaches to developing new efficient catalysts. Herein, the effects of S-doping on melon-based carbon nitride (CN) for the photocatalytic selective oxygen reduction reaction (ORR) have been comprehensively investigated by first-principles calculations. The configurations, electronic properties, optical properties, and the reaction performance of the S-doped melon-based CN have been studied and discussed. The results demonstrate that the decoration with S atoms exhibited substantial effects, involving the redistribution of the charge density and tuning of the bandgap, which promote the photocatalytic selective ORR activity. Accordingly, O2 is activated on the S-doped system with about 0.4 e of charge obtained from catalytic surfaces, leading to the thermodynamically feasible H2O2 and H2O formation, which is in good agreement with the experimental results. Our results provide theoretical insights into the design and development of polymeric carbon nitride (PCN) as well as other metal-free photocatalysts for the selective ORR. |
| Databáze: | OpenAIRE |
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