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Weak-Field Electro-Flash Induced Asymmetric Catalytic Sites toward Efficient Solar Hydrogen Peroxide Production.
Chen, Fangshuai; Lv, Ximeng; Wang, Haozhen; Wen, Fan; Qu, Liangti; Zheng, Gengfeng; Han, Qing.
Afiliação
  • Chen F; Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, P. R. China.
  • Lv X; Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Faculty of Chemistry and Materials Science, Fudan University, Shanghai 200438, P. R. China.
  • Wang H; Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Faculty of Chemistry and Materials Science, Fudan University, Shanghai 200438, P. R. China.
  • Wen F; Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, P. R. China.
  • Qu L; Key Laboratory of Organic Optoelectronics & Molecular Engineering of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing 100084, P. R. China.
  • Zheng G; Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Faculty of Chemistry and Materials Science, Fudan University, Shanghai 200438, P. R. China.
  • Han Q; Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Faculty of Chemistry and Materials Science, Fudan University, Shanghai 200438, P. R. China.
JACS Au ; 4(3): 1219-1228, 2024 Mar 25.
Article em En | MEDLINE | ID: mdl-38559724
ABSTRACT
Borocarbonitride (BCN), in a mesoscopic asymmetric state, is regarded as a promising photocatalyst for artificial photosynthesis. However, BCN materials reported in the literature primarily consist of symmetric N-[B]3 units, which generate highly spatial coupled electron-hole pairs upon irradiation, thus kinetically suppressing the solar-to-chemical conversion efficiency. Here, we propose a facile and fast weak-field electro-flash strategy, with which structural symmetry breaking is introduced on key nitrogen sites. As-obtained double-substituted BCN (ds-BCN) possesses high-concentration asymmetric [B]2-N-C coordination, which displays a highly separated electron-hole state and broad visible-light harvesting, as well as provides electron-rich N sites for O2 affinity. Thereby, ds-BCN delivers an apparent quantum yield of 7.6% at 400 nm and a solar-to-chemical conversion efficiency of 0.3% for selective 2e-reduction of O2 to H2O2, over 4-fold higher than that of the traditional calcined BCN analogue and superior to the metal-free C3N4-based photocatalysts reported so far. The weak-field electro-flash method and as-induced catalytic site symmetry-breaking methodologically provide a new method for the fast and low-cost fabrication of efficient nonmetallic catalysts toward solar-to-chemical conversions.

Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2024 Tipo de documento: Article

Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2024 Tipo de documento: Article