Tandem Synthesis of Biobased Nylon Monomer via Dynamic Hydrogen Management through Medium Entropy Alloy

The synthesis of 2,5-bis(aminomethyl)furan (BAMF) from 5-hydroxymethylfurfural (5-HMF) offers a biobased diamine monomer for establishing a low-carbon nylon industrial chain. However, this one-pot tandem reaction is hindered by imbalanced dehydrogenation/hydrogenation kinetics. Herein, we proposed a dynamic hydrogen management strategy by coupling hydrogen storage with dehydrogenation/hydrogenation in a CuNiCoGa medium-entropy alloy (MEA) catalyst. The MEA’s atomic-level dispersion of multifunctional sites facilitates H* migration from CuNiCo to Ga, temporarily stabilizing intermediates as Ga–H bonds to facilitate dehydrogenation. Subsequent imine formation triggers spontaneous Ga–H dissociation, driven by hydrogen concentration gradients, to enable efficient hydrogenation. Hence, the CuNiCoGa-MEA catalyst achieves 99% BAMF yield, surpassing the 22.1% yield of Ga-free CuNiCo MEA. By copolymerizing rigid BAMF with flexible dodecanedioic acid, we pioneer a thermally stable polyamide complementing biobased nylon. This work establishes an integrated polyamide production through bioderived feedstocks, catalytic innovation, and process intensification, aligning with circular economy principles and low carbon emissions.