Breaking through water-splitting bottlenecks over carbon nitride with fluorination

Graphitic carbon nitride has long been considered incapable of splitting water molecules into hydrogen and oxygen without adding small molecule organics despite the fact that the visible-light response and proper band structure fulfills the proper energy requirements to evolve oxygen. Herein, throug...

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Bibliographic Details
Published in:Nature communications 2022-11, Vol.13 (1), p.6999-6999, Article 6999
Main Authors: Wu, Ji, Liu, Zhonghuan, Lin, Xinyu, Jiang, Enhui, Zhang, Shuai, Huo, Pengwei, Yan, Yan, Zhou, Peng, Yan, Yongsheng
Format: Article
Language:English
Subjects:
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Carbon
Carbon nitride
Catalysts
Chemical bonds
Density functional theory
Energy requirements
Evolution
Fluorination
Fluorine
Humanities and Social Sciences
Hydrogen evolution
Light effects
multidisciplinary
Oxygen
Oxygen evolution reactions
Science
Science (multidisciplinary)
Splitting
Water chemistry
Water splitting
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Summary:Graphitic carbon nitride has long been considered incapable of splitting water molecules into hydrogen and oxygen without adding small molecule organics despite the fact that the visible-light response and proper band structure fulfills the proper energy requirements to evolve oxygen. Herein, through in-situ observations of a collective C = O bonding, we identify the long-hidden bottleneck of photocatalytic overall water splitting on a single-phased g-C 3 N 4 catalyst via fluorination. As carbon sites are occupied with surface fluorine atoms, intermediate C=O bonding is vastly minimized on the surface and an order-of-magnitude improved H 2 evolution rate compared to the pristine g-C 3 N 4 catalyst and continuous O 2 evolution is achieved. Density functional theory calculations suggest an optimized oxygen evolution reaction pathway on neighboring N atoms by C–F interaction, which effectively avoids the excessively strong C-O interaction or weak N-O interaction on the pristine g-C 3 N 4 . Graphitic carbon nitride has long been considered a poor oxygen evolution catalyst. Here, the authors report a simple fluorination strategy to prevent the accumulation of inert C=O on carbon nitride to break through this bottleneck.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-022-34848-8