Synergistic NiCo Bimetallic Oxides for Electrocatalytic Upcycling of Polylactic Acid to Acetate With In Situ Mechanistic Insights

Polylactic acid is currently the most widely produced biodegradable polyester plastic. However, its conventional disposal methods such as natural degradation, composting, and incineration not only generate substantial CO 2 emissions but also result in significant resource loss. In contrast, upcycling technologies can transform plastic waste into high value‐added chemicals, offering considerable application potential in producing renewable monomers for new polymers, sustainable fuels, and value‐added fine chemicals for the pharmaceutical and chemical industries. In this study, we fabricated a self‐supported NiCo bimetallic oxides (NiCoO x /NF) electrode via an electrodeposition strategy for the electrocatalytic upcycling of PLA wastes. Owing to the abundant exposure of active sites and efficient electron transfer between bimetallic species, the electrode exhibited excellent electrocatalytic performance, enabling the electrocatalytic reforming of PLA hydrolysates into acetate with Faradaic efficiencies exceeding 90% in the potential range of 1.32–1.52 V. In situ characterizations identified pyruvate and CH 3 CO‐ as key intermediates mediating the formation of acetate. Furthermore, techno‐economic analysis demonstrated the scalability and profitability of this approach. This work provides a novel and sustainable pathway for the green and efficient utilization of PLA wastes.