Kinetically controlled proton removal via bio-inspired hybrid bilayer membrane functionalized electrode for ethylene...

As a cornerstone of the circular carbon economy, the upcycling of polyethylene terephthalate (PET) relies on efficient monomer recovery and subsequent high-value transformation. While PET can be effectively broken down into ethylene glycol (EG) via scalable depolymerization techniques such as hydrolysis, alcoholysis, or pyrolysis, the subsequent electrochemical ethylene glycol oxidation reaction (EgOR) faces a significant selectivity bottleneck. This reaction is governed by complex proton-coupled electron transfer (PCET) pathways that typically favor C-C bond cleavage, resulting in low-value C1 products like formic acid and CO₂. In this work, we overcome these limitations by employing a bio-inspired hybrid bilayer membrane (HBM) functionalized electrode to exert kinetic control over the proton removal rate. By precisely modulating the electrocatalytic microenvironment at the electrode interface, the HBM suppresses over-oxidation and steers the reaction toward the targeted generation of C2 products. We demonstrate the selective production of glycolic acid, a premium chemical in the cosmetics industry with a market value exceeding 25 times that of the EG feedstock. These results establish that regulating the kinetics of proton transfer via HBM technology is a transformative strategy for controlling reaction selectivity in complex oxidation pathways. This approach offers a potentially scalable, renewable-energy-powered route for upcycling plastic waste derivatives into high-value chemical outputs, providing significant translational value for sustainable resource recovery.