Weak-Field Electro-Flash Induced Asymmetric Catalytic Sites toward Efficient Solar Hydrogen Peroxide Production
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,...
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Published in | JACS Au Vol. 4; no. 3; pp. 1219 - 1228 |
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Main Authors | , , , , , , |
Format | Journal Article |
Language | English |
Published |
United States
American Chemical Society
25.03.2024
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Subjects | |
Online Access | Get full text |
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Summary: | 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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Bibliography: | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
ISSN: | 2691-3704 2691-3704 |
DOI: | 10.1021/jacsau.4c00076 |