Efficient Polyethylene Furanoate Synthesis From CO₂ and 5-(Hydroxymethyl)furfural

The sustainable synthesis of polyethylene furanoate (PEF) from waste-derived CO₂ and 5-(hydroxymethyl)furfural (HMF) is limited by kinetic mismatches, pH incompatibility, and stoichiometric imbalances in conventional cascade electrolysis systems. Herein, we propose a reaction-pair recombination strategy that decouples key redox steps and selectively reintegrates them within a three-cell cascade system. This configuration enables simultaneous generation of ethylene glycol (EG) and furandicarboxylic acid (FDCA) at industrial-level current densities with Faradaic efficiencies of 71.5% and 87.1%, respectively, achieving a near-optimal EG:FDCA ratio of 3:1. During a stable operation period of 25 h, the three-cell cascade system exhibited a bis(2-hydroxyethyl) furan-2,5-dicarboxylate (BHEF) productivity of 28.4 mmol L^-1 h^-1 and a PEF production rate of 2.1 g day^-1. Compared with the conventional routes, the new pathway achieves nearly 50-fold higher energy efficiency and a low global warming potential of 0.83 g_CO2-eq per gram of PEF, providing a sustainable platform for waste valorization into high-value polymers.