Mechanochemical Ball Milling Achieves Green and Ultrahighly Efficient Recycling of Lithium-Ion Batteries.

With the increasing application of lithium-ion batteries (LIBs), the green and efficient recycling of spent LIBs has become a global priority. However, current techniques share common drawbacks such as low cost-effectiveness, harsh operating conditions, and overlooking of post-treatment environmental hazards. Herein, we propose a green mechanochemical strategy that utilizes the electrons and reactive oxygen species generated by ball milling to achieve ultrahighly efficient metal recovery and removal of residual organic pollutants. The recovery efficiencies from lithium manganese oxide (LMO) batteries reached ∼100% for lithium and 94.3% for manganese within 60 min, and the representative residual organic pollutants were effectively removed, ranging from 73.1 to 99.1%. Similar efficiencies were achieved for lithium iron phosphate and nickel manganese cobalt batteries. The generation of abundant electrons and reactive oxygen species during the ball milling process is proposed as the main mechanism underlying the efficient metal recovery and pollutant degradation. The effective reduction in the valence state of manganese in the LMO powders was verified by X-ray adsorption fine structure spectroscopy. The excellent performance of our strategy in Li recovery and mitigating environmental hazards has far surpassed those of existing techniques and demonstrates the exceptional potential of mechanochemical ball milling as a green technique for LIB recycling.