General Formation of Interfacial Assembled Hierarchical Micro-Nano Arrays for Biomass Upgrading-Coupled Hydrogen Production

Construction of efficient catalysts to couple biomass upgrading with hydrogen production is significant for improving energy efficiency, which remains a challenge. Herein, a general method for manufacturing 3D hierarchical micro-nano arrays consisting of template framework and nanoparticle-decorated nanosheets is reported. This strategy provides an opportunity to controllably tailor the interfacial assembly of nanosheets on precursor template materials. The obtained Co@NiMoO-Ni/NF exhibits enhanced electrocatalytic performance for biomass oxidation and hydrogen production. It only needs 1.21 V to achieve 10 mA cm-2 for 5-hydroxymethylfurfural electrooxidation reaction (HMFOR) assisted H2 evolution reaction (HER). The good catalytic performance is ascribed to the intense interaction between template (Co) and nanoparticle-decorated nanosheets (NiMoO-Ni), which tunes the electron structure of the catalyst to optimize the adsorption behavior of HMFOR/HER intermediates and promote the bonds breakage of key intermediates in the HMFOR/HER process. This work thus provides a strategy for designing ideal catalysts for biomass upgrading-coupled H2 production. Co@NiMoO-Ni/NF is constructed as an efficient bifunctional catalyst for 5-hydroxymethylfurfural electrooxidation reaction (HMFOR) and hydrogen evolution reaction (HER). Experiments and theoretical calculations reveal that the interaction between Co and NiMoO-Ni optimizes the adsorption behavior of HMFOR/HER intermediates and promotes the bond breakage of key intermediates in the catalytic process, thus enhancing the catalytic activity.image