A win-win recycling strategy for spent lithium-ion batteries: Prioritized selective lithium extraction afterwards triggers intrinsic catalysis

Achieving highly efficient and environmentally friendly recycling of spent lithium-ion batteries (LIBs) is crucial for addressing the growing demand for environmental and resource sustainability challenges. In this study, a win-win recycling strategy for spent LIBs is proposed, involving selective high-yield Li extraction from spent ternary cathode materials (NCM, LiNi_xCo_yMn_zO₂), followed by the activation of intrinsic catalytic properties for the degradation of volatile organic compounds (VOCs). Treatment of NCM111 (LiNi_xCo_yMn_zO₂, x,y,z = 1/3) via copper sulfate-assisted thermal reconstruction enabled selective Li extraction through water leaching, achieving a Li recovery rate of 98.03%; and subsequent purification and precipitation processes yielded Li₂CO₃. The intrinsic catalytic activity of the leaching residue, activated after selective Li recovery through aqueous leaching, was subsequently utilized as a catalyst (NCM-Cu/13X) for the efficient oxidative degradation of gaseous toluene, achieving a removal efficiency exceeding 99.5%. This mutually beneficial strategy enhances atom economy through the incorporation of copper sulfate, which not only facilitates Li extraction but also promotes structural and surface modifications of the catalyst. Experimental characterizations combined with density functional theory (DFT) calculations demonstrate the enhanced formation of oxygen vacancies (O_V) and surface-adsorbed oxygen (O_ads) on the catalyst surface, thereby promoting the catalytic degradation of toluene. Life cycle assessment (LCA) demonstrates that this technology entails manageable ecological impacts while providing net environmental benefits, underscoring its potential as a sustainable solution for LIBs recycling. © 2026 Published by Elsevier B.V.