Issue 37, 2022

Electrocatalytic valorization of 5-hydroxymethylfurfural coupled with hydrogen production using tetraruthenium-containing polyoxometalate-based composites

Abstract

Electrocatalytic biomass valorization represents a promising route to produce sustainable and carbon-neutral products, especially when coupled with hydrogen production. Here we report a Ru4/PEI-rGO electrocatalyst, prepared by electrostatic integration of a tetraruthenium-containing polyoxometalate, Rb8K2[Ru4(μ-O)4(μ-OH)2(H2O)4(γ-SiW10O36)2]·25H2O (Ru4), with polyethyleneimine (PEI) modified rGO, which can efficiently electrocatalyze biomass-derived 5-hydroxymethylfurfural (HMF) to value-added furanic products simultaneously coupled with H2 production in near neutral media. Under minimally optimized conditions, the conversion of HMF and the yield of H2 reached 50.8% and 55.4 μmol after 6 hour electrocatalysis at 0.94 V vs. Ag/AgCl, respectively. 2,5-Diformylfuran (DFF) was detected as the dominant oxidation product with a selectivity of 66.2%. The faradaic efficiencies (FEs) of the anode and cathode reached 97.0 ± 3% and 100.2 ± 2%, respectively. In the presence of the 2,2,6,6-tetramethylpiperidinyloxyl (TEMPO) additive, the conversion of HMF reached 99.7%, and the distribution of the oxidation product has been greatly altered, wherein furanic carboxyl products are dominant. Various electrochemical characterization studies and spectrogram analyses, especially Fourier Transformed Alternating Current (FTAC) voltammetry, were employed to disclose that RuV centers were catalytically active species, and the three-electron oxidized Ru4 species are responsible for the excellent electrocatalytic activity. Long-term electrocatalysis demonstrated that the present Ru4/PEI-rGO composite possessed good stability for catalysis.

Graphical abstract: Electrocatalytic valorization of 5-hydroxymethylfurfural coupled with hydrogen production using tetraruthenium-containing polyoxometalate-based composites

Supplementary files

Article information

Article type
Paper
Submitted
18 mar 2022
Accepted
20 iyn 2022
First published
20 iyn 2022

J. Mater. Chem. A, 2022,10, 19963-19971

Electrocatalytic valorization of 5-hydroxymethylfurfural coupled with hydrogen production using tetraruthenium-containing polyoxometalate-based composites

H. Zhou, Y. Dong, X. Xin, M. Chi, T. Song and H. Lv, J. Mater. Chem. A, 2022, 10, 19963 DOI: 10.1039/D2TA02148J

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