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Rejoint of Carbon Nitride Fragments into Multi‐Interfacial Order‐Disorder Homojunction for Robust Photo‐Driven Generation of H<sub>2</sub>O<sub>2</sub>

Fengting He, Yang‐Ming Lu, Yuzhao Wu, Shuling Wang, Yang Zhang, Pei Dong, Yongqiang Wang, Chaocheng Zhao, Shuaijun Wang, Jinqiang Zhang, Shaobin Wang

2023Advanced Materials142 citationsDOIOpen Access PDF

Abstract

Abstract Photocatalytic technology based on carbon nitride (C 3 N 4 ) 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, a novel approach is devised by fragmenting bulk C 3 N 4 into smaller pieces (CN‐NH 4 ) and then 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 boost charge dynamics and facilitate more spatially and orderly separated redox centers. As a result, CN‐NH 4 ‐NaK demonstrates 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 (&gt; 91%), and a prominent solar‐to‐chemical conversion efficiency exceeding 2.3%. These remarkable results surpass pristine C 3 N 4 by 158 times and outperform 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.

Topics & Concepts

HomojunctionMaterials scienceCarbon nitrideNitrideCarbon fibersYield (engineering)PhotocatalysisRedoxNanotechnologyChemical engineeringCatalysisOptoelectronicsChemistryHeterojunctionOrganic chemistryEngineeringComposite numberLayer (electronics)MetallurgyComposite materialAdvanced Photocatalysis TechniquesElectronic and Structural Properties of OxidesCopper-based nanomaterials and applications