Highly Efficient Electro‐reforming of 5‐Hydroxymethylfurfural on Vertically Oriented Nickel Nanosheet/Carbon Hybrid Catalysts: Structure–Function Relationships

Abstract Ni‐promoted electrocatalytic biomass reforming has shown promising prospect in enabling high value‐added product synthesis. Here, we developed a novel hybrid catalyst with Ni nanosheet forests anchored on carbon paper. The hybrid catalyst exhibits high efficiency in electrooxidation of HMF to FDCA coupling with H 2 production in high purity. The Ni nanosheets have small crystal grain sizes with abundant edges, which is able to deliver an efficient HMF oxidation to FDCA (selectivity >99 %) at low potential of 1.36 V RHE with high stability. The post‐reaction structure analysis reveals the Ni nanosheets would transfer electrons to carbon and readily turn into NiO x and Ni(OH) x during the reaction. DFT results suggest high valence Ni species would facilitate the chemical adsorption (activation) of HMF revealing the reaction pathway. This work emphasizes the importance of the precise control of Ni activity via atomic structure engineering.