Dual‐Site Synergistic Electrocatalysis Enables Highly Selective Upcycling of Real‐World Plastic Waste to Glycolic Acid

Abstract

Abstract Plastic waste pollution presents a critical environmental challenge, with polyethylene terephthalate (PET) among the most prevalent and persistent forms of plastic waste. This study develops a sustainable electrocatalytic strategy to upcycle PET‐derived ethylene glycol (EG) into high‐value glycolic acid (GA) using Ni─Fe dual single‐atom catalysts (Ni 1 ─Fe 1 ─N─C DSACs). By optimizing the binding energies of *EG and *OH through dual‐site synergy, the catalysts achieve a Faradaic efficiency of 96.1% and selectivity above 90% for GA production. Mechanistic insights reveal that oxygen‐affine Ni atoms facilitate *OH generation, enhancing EG oxidation while preventing over‐oxidation. The technology is demonstrated in a membrane electrode assembly (MEA) flow electrolyzer, achieving stable electrolysis for over 100 h with a Faradaic efficiency exceeding 85%. A life cycle assessment (LCA) confirms that electrocatalytic reforming outperforms mechanical recycling and incineration across multiple environmental and economic indicators, significantly reducing carbon emissions, enhancing resource efficiency, and ensuring greater process stability. These findings highlight the potential of electrocatalytic PET upcycling as a scalable and environmentally sustainable solution for addressing plastic pollution and advancing circular economy goals.