Weak-Field Electro-Flash Induced Asymmetric Catalytic Sites toward Efficient Solar Hydrogen Peroxide Production.
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.
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MEDLINE
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En
Ano de publicação:
2024
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Article