期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 48, 页码 25546-25550出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202111769
关键词
abundant edge active sites; H2O2 production; oxygen reduction reaction; photocatalysts; polymeric carbon nitride
资金
- National Key Plan for Research and Development of China [2016YFC0502203]
- Natural Science Foundation of China [51979081]
- Fundamental Research Funds for the Central Universities [B200202103, B210202052]
- China Postdoctoral Science Foundation [2020M680063, 2021T140176]
- National Science Funds for Creative Research Groups of China [51421006]
- PAPD
The TP-PCN photocatalyst with abundant edge active sites exhibits superior H2O2 generation rate, providing a new strategy for designing efficient photocatalysts. Furthermore, DFT calculations suggest that TP-PCN is more favorable for electron transiting, optimizing O-2 activation and reducing the energy barrier of H2O2 formation.
Polymeric carbon nitride (PCN) as a class of two-electron oxygen reduction reaction (2 e(-) ORR) photocatalyst has attracted much attention for H2O2 production. However, the low activity and inferior selectivity of 2 e(-) ORR greatly restrict the H2O2 production efficiency. Herein, we develop a new strategy to synthesize hydrophilic, fragmented PCN photocatalyst by the terminating polymerization (TP-PCN) effect of iodide ions. The obtained TP-PCN with abundant edge active sites (AEASs), which can form quasi-homogeneous photocatalytic system, exhibits superior H2O2 generation rate (3265.4 mu M h(-1)), far surpassing PCN and other PCN-based photocatalysts. DFT calculations further indicate that TP-PCN is more favorable for electron transiting from beta spin-orbital to the pi* orbitals of O-2, which optimizes O-2 activation and reduces the energy barrier of H2O2 formation. This work provides a new concept for designing functional photocatalysts and understanding the mechanism of O-2 activation in ORR for H2O2 production.
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