Surface fluorination of BiVO4 for the photoelectrochemical oxidation of glycerol to formic acid

Yang Liu, Huishan Shang, Bing Zhang, Dongpeng Yan () and Xu Xiang ()
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Yang Liu: Beijing University of Chemical Technology
Huishan Shang: Zhengzhou University
Bing Zhang: Zhengzhou University
Dongpeng Yan: Beijing Normal University
Xu Xiang: Beijing University of Chemical Technology

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract The C–C bond cleavage of biomass-derived glycerol to generate value-added C1 products remains challenging owing to its slow kinetics. We propose a surface fluorination strategy to construct dynamic dual hydrogen bonds on a semiconducting BiVO4 photoelectrode to overcome the kinetic limit of the oxidation of glycerol to produce formic acid (FA) in acidic media. Intensive spectroscopic characterizations confirm that double hydrogen bonds are formed by the interaction of the F–Bi–F sites of modified BiVO4 with water molecules, and the unique structure promotes the generation of hydroxyl radicals under light irradiation, which accelerates the kinetics of C–C bond cleavage. Theoretical investigations and infrared adsorption spectroscopy reveal that the double hydrogen bond enhances the C=O adsorption of the key intermediate product 1,3-dihydroxyacetone on the Bi–O sites to initiate the FA pathway. We fabricated a self-powered tandem device with an FA selectivity of 79% at the anode and a solar-to-H2 conversion efficiency of 5.8% at the cathode, and these results are superior to most reported results in acidic electrolytes.

Date: 2024
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DOI: 10.1038/s41467-024-52161-4

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