Electrocatalytic conversion of biomass platform chemicals to jet fuel precursors is a promising approach to alleviate the energy crisis caused by the excessive exploitation and consumption of non-renewable fossil fuels. However, an aqueous electrolyte has been rarely studied. In this study, we demonstrate an anodic electrocatalysis route for producing jet fuel precursors from biomass platform chemicals on Ni-based electrocatalysts in an aqueous electrolyte at room temperature and atmosphere pressure. The desired product exhibited high selectivity for the jet fuel precursor (95.4%) and an excellent coulombic efficiency of 210%. A series of characterizations demonstrated that Ni species were the active sites for the coupling process. In addition, the coupling reaction could be achieved by generating radical cations and inhibiting the side reaction. First, the electrochemical process could activate the furfural (FF) molecule and generate radical cations, resulting in an average of 2.0 times chain propagation. The levulinic acid (LA) molecules played a vital role in the coupling reaction. The adsorption strength of LA on NiN was higher than that of FF, which could inhibit the side reaction (the oxidation of FF) and achieve high selectivity. Meanwhile, the LA molecules were adsorbed on the NiN surface and then disrupted the formation of Ni species, thus favoring the coupling reaction. This work demonstrates an efficient route to produce jet fuel precursors directly from biomass platform chemicals and provides a comprehensive understanding of the anodic coupling process.
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http://dx.doi.org/10.1021/jacs.2c11153 | DOI Listing |
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