Photocatalytic technology based on carbon nitride (C N ) offers a sustainable and clean approach for hydrogen peroxide (H O ) production, but the yield is severely limited by the sluggish hot carriers due to the weak internal electric field. In this study, a novel approach is devised by fragmenting bulk C N into smaller pieces (CN-NH ) and then subjecting it to a directed healing process to create multiple order-disorder interfaces (CN-NH -NaK). The resulting junctions in CN-NH -NaK significantly boost charge dynamics and facilitate more spatially and orderly separated redox centers. As a result, CN-NH -NaK demonstrates outstanding photosynthesis of H O via both two-step single-electron and one-step double-electron oxygen reduction pathways, achieving a remarkable yield of 16675 µmol h g , excellent selectivity (> 91%), and a prominent solar-to-chemical conversion efficiency exceeding 2.3%. These remarkable results surpass pristine C N by 158 times and outperform previously reported C N -based photocatalysts. This work represents a significant advancement in catalyst design and modification technology, inspiring the development of more efficient metal-free photocatalysts for the synthesis of highly valued fuels.
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http://dx.doi.org/10.1002/adma.202307490 | DOI Listing |
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