Rejoint of Carbon Nitride Fragments into Multi-Interfacial Order-Disorder Homojunction for Robust Photo-Driven Generation of H 2 O 2 .

Photocatalytic technology based on carbon nitride offers a sustainable and clean approach for hydrogen peroxide (H 2 O 2 ) production, but the yield is severely limited by the sluggish hot carriers due to the weak internal electric field. In this study, we devised a novel approach by fragmenting graphitic carbon nitride into smaller pieces (CN-NH 4 ), followed by subjecting it to a directed healing process to create multiple order-disorder interfaces (CN-NH 4 -NaK). The resulting junctions in CN-NH 4 -NaK significantly boosted charge dynamics and facilitated more spatially and orderly separated redox centers. As a result, CN-NH 4 -NaK demonstrated outstanding photosynthesis of H 2 O 2 via both two-step single-electron and one-step double-electron oxygen reduction pathways, achieving a remarkable yield of 16675 μmol h -1  g -1 , excellent selectivity (> 91%), and a prominent solar-to-chemical conversion efficiency exceeding 2.3%. These remarkable results surpassed pristine C 3 N 4 by 158 times and outperformed previously reported C 3 N 4 -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. This article is protected by copyright. All rights reserved.