From Battery Waste to Electrocatalyst: Topological Disorder-Driven Upcycling of Spent LiCoO2 for Selective H2O2 Electrosynthesis.

The large-scale deployment of lithium-ion batteries has led to a rapid increase in spent cathode materials, creating unprecedented challenges for their sustainable management. Herein, we report a direct structural upgrading strategy that converts spent lithium cobalt oxide (LiCoO2) into an efficient electrocatalyst for the two-electron oxygen reduction reaction (2e- ORR). The optimized catalyst exhibits markedly enhanced activity (210 mA cm-2) and selectivity (∼96%) toward hydrogen peroxide (H2O2) generation under alkaline conditions. We reveal that disorder-induced distortions of CoO6 octahedra reconstruct the local crystal field, stabilize high-spin Co centers, and strengthen d-π* spin coupling and Co-O covalency. This cooperative orbital-spin modulation optimizes *OOH adsorption while energetically suppressing *OH--mediated four-electron ORR pathways. This work demonstrates the feasibility of directly upgrading spent LiCoO2 cathodes into high-performance electrocatalysts, offering insights for the rational reutilization of structurally robust battery materials.