Redox‐Mediated Electrified Method for Green and Low‐Cost Spent Lithium‐Ion Battery Materials Recycling

ABSTRACT After 30 years of commercialization and mass production, lithium‐ion batteries have generated massive waste streams, especially with their expanding use in electric vehicles. Recycling spent batteries and valorizing useful components are therefore increasingly urgent for sustainable development. However, conventional pyrometallurgical and hydrometallurgical methods are limited by high energy consumption or large chemical input, creating demand for greener and more efficient recycling technologies. Here, using LiCoO 2 as an example, we report a closed‐loop electrified chemical process based on redox‐targeting reactions to recover valuable species from spent battery materials using only electricity and water. Complementary reductive leaching of LiCoO 2 and oxidative leaching of LiFePO 4 were performed with anthraquinone‐2,7‐disulfonate as a regenerative redox mediator to sequentially break down LiCoO 2 and achieve efficient separation of Co 2+ and Li + in the form of Co(OH) 2 and LiOH. This cost‐effective and environmentally friendly method was also extended to the recycling of LiNi x Mn y Co z O 2 with a high recovery rate of Li + and transition metal species. It is anticipated that the electrified chemical recycling method demonstrated here would provide a credible solution to the valorization of battery waste and contribute to the sustainable development of lithium‐ion batteries.