A Highly General Potential‐Gating Strategy for Electrocatalytic Upcycling of Waste Polyester Plastics

ABSTRACT

Electrocatalytic upcycling of waste polyester plastics driven by renewable electricity offers a sustainable route for resource utilization, yet its practical implementation is hampered by the poor selectivity control stemming from the inherent complex monomer of polyesters. Herein, we propose a potential‐gating principle for the selectivity‐controllable upcycling of α,ω‐diols and hydroxy acids—the most pivotal monomers of polyester—and design a potential‐gated PVP‐Pd‐Ni(OH) ₂ ‐CV/NF catalyst. This catalyst enables precise manipulation of product distribution simply by switching the applied potential without the need for catalyst replacement, while demonstrating broad applicability to seven polyesters. Moreover, the composite catalyst exhibits a sevenfold activity enhancement over the Pd/NF benchmark. Mechanistic investigations reveal that the adsorption behavior of hydroxy acid intermediates is the key selectivity‐determining step. Sequential electrolysis of real post‐consumer polyester hydrolysates over four stages for 198 h retains high target product selectivity (84%–98%), thus showcasing a general and sustainable route for plastic waste recycling.