Weak-Field Electro-Flash Induced Asymmetric Catalytic Sites toward Efficient Solar Hydrogen Peroxide Production

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. Asobtained 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 O 2 affinity. Thereby, ds-BCN delivers an apparent quantum yield of 7.6% at 400 nm and a solar-tochemical conversion efficiency of 0.3% for selective 2e-reduction of O 2 to H 2 O 2 , over 4-fold higher than that of the traditional calcined BCN analogue and superior to the metal-free C 3 N 4 -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.