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>.
basic_science · Level V
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- Record sourced from PubMed, PMID 37939231.
- Also identified by DOI 10.1002/adma.202307490.
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Abstract
Photocatalytic technology based on carbon nitride (C<sub>3</sub> N<sub>4</sub> ) offers a sustainable and clean approach for hydrogen peroxide (H<sub>2</sub> O<sub>2</sub> ) 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<sub>3</sub> N<sub>4</sub> into smaller pieces (CN-NH<sub>4</sub> ) and then subjecting it to a directed healing process to create multiple order-disorder interfaces (CN-NH<sub>4</sub> -NaK). The resulting junctions in CN-NH<sub>4</sub> -NaK significantly boost charge dynamics and facilitate more spatially and orderly separated redox centers. As a result, CN-NH<sub>4</sub> -NaK demonstrates outstanding photosynthesis of H<sub>2</sub> O<sub>2</sub> via both two-step single-electron and one-step double-electron oxygen reduction pathways, achieving a remarkable yield of 16675 µmol h<sup>-1</sup> g<sup>-1</sup> , excellent selectivity (> 91%), and a prominent solar-to-chemical conversion efficiency exceeding 2.3%. These remarkable results surpass pristine C<sub>3</sub> N<sub>4</sub> by 158 times and outperform previously reported C<sub>3</sub> N<sub>4</sub> -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.