Breaking through water-splitting bottlenecks over carbon nitride with fluorination

Ji Wu, Zhonghuan Liu, Xinyu Lin, Enhui Jiang, Shuai Zhang, Pengwei Huo, Yan Yan (), Peng Zhou () and Yongsheng Yan
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Ji Wu: Jiangsu University
Zhonghuan Liu: Jiangsu University
Xinyu Lin: Jiangsu University
Enhui Jiang: Jiangsu University
Shuai Zhang: Jiangsu University
Pengwei Huo: Jiangsu University
Yan Yan: Jiangsu University
Peng Zhou: University of Michigan
Yongsheng Yan: Jiangsu University

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract 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-C3N4 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 H2 evolution rate compared to the pristine g-C3N4 catalyst and continuous O2 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-C3N4.

Date: 2022
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DOI: 10.1038/s41467-022-34848-8

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