Spent Battery-to-Catalyst: Asymmetric Mn-O Motifs Boost Oxygen Activation for Upgrading Polystyrene to Aromatic Oxygenates.

Zhang, Shuyi; Chu, Mingyu; Zhang, Qingqing; Jiao, Binglei; Cao, Muhan; Xu, Panpan; Zhang, Qiao; Chen, Jinxing · ACS Nano · 2026

basic_science · Level V

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Abstract

The rapid expansion of global lithium-ion battery production has positioned spent batteries as a critical challenge in resource sustainability and environmental stewardship. Breaking from conventional recycling paradigms that focus solely on metal ion/oxide recovery, this study pioneers an innovative inorganic-organic solid waste co-recycling system. We demonstrate the catalytic potential of spent lithium manganese oxide (LMO) materials through their good oxidation properties to upcycle waste polystyrene (PS) into value-added benzoic acid (BA). Mechanistic investigations reveal that Li<sup>+</sup> polarization induces asymmetric Mn<sup>3+</sup>-O-Mn<sup>4+</sup> coordination in the LMO structure, facilitating lattice oxygen activation and oxygen vacancy formation. These structural modifications enable efficient O<sub>2</sub> conversion into reactive superoxide radicals (<sup>•</sup>O<sub>2</sub><sup>-</sup>), which drive the selective oxidative cleavage of PS chains. The optimized system achieves an exceptional 88% solid conversion with ∼70% BA selectivity at a low temperature of 150 °C within 1 h. The dual waste-stream remediation approach demonstrates significant potential for sustainable resource recovery at the energy-environment nexus.