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>

Authors: Fengting He, Yangming Lu, Yuzhao Wu, Shuling Wang, Yang Zhang, Pei Dong, Yongqiang Wang, Chaocheng Zhao, Shuaijun Wang, Jinqiang Zhang, Shaobin Wang

Published: 2023-11-08

DOI: 10.1002/adma.202307490

Source: Full article


Abstract

AbstractPhotocatalytic technology based on carbon nitride (C3N4) offers a sustainable and clean approach for hydrogen peroxide (H2O2) 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 C3N4 into smaller pieces (CN‐NH4) and then subjecting it to a directed healing process to create multiple order‐disorder interfaces (CN‐NH4‐NaK). The resulting junctions in CN‐NH4‐NaK significantly boost charge dynamics and facilitate more spatially and orderly separated redox centers. As a result, CN‐NH4‐NaK demonstrates outstanding photosynthesis of H2O2 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 surpass pristine C3N4 by 158 times and outperform previously reported C3N4‐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.