Efficient Direct Recycling of Lithium-Ion Battery Cathodes by Targeted Healing

Recycling of spent lithium-ion batteries (LIBs) is an urgent need to address their environmental and global sustainability issues. Here, we report an efficient and environmentally benign LIB regeneration method based on defect-targeted healing, which represents a paradigm-shift LIB recycling strategy. Specifically, by combining low-temperature aqueous solution relithiation and rapid post-annealing, we demonstrate successful direct regeneration of spent LiFePO4 (LFP) cathodes, one of the most important materials for EVs and grid storage applications. We show revitalization of composition, structure, and electrochemical performance of LFP with various degradation conditions to the same levels as the pristine LFP. Life-cycle analysis of different LIB recycling processes shows that this defect-targeted direct reycling approach can significantly reduce energy usage and greenhouse gas (GHG) emissions, leading to more economic and environmental benefits compared with today’s hydrometallurgical and pyrometallurgical methods. [Display omitted] •A safe and low-cost method was developed to directly recycle LiFePO4 cathodes•A targeted healing strategy can fully resolve composition and structure defects•The regenerated cathode reached the same performance of pristine LiFePO4 materials•Direct recycling shows dramatically improved economic and environmental benefits The consumption of lithium-ion batteries is experiencing booming growth in the modern industry due to their widespread applications. With billions of batteries reaching their lifetime soon, significant concerns on the economic and environmental issues have been raised about how to treat these spent batteries so that our society will not face similar crisis incurred in the case of plastic wastes. However, traditional technologies used in today’s recycling industry are limited to recovering expensive metals through energy-intensive processes, which cause significant greenhouse gas emissions and secondary wastes, posing additional environmental concerns. To tackle this challenge, we developed a safe, low-cost, and efficient direct recycling approach that is based on targeted healing. This paradigm-shift method leverages our understanding on phase and structure evaluations of the LIB cathode and produces ready-to-use recycled cathode materials that match the electrochemical performance of pristine materials. A paradigm-shift lithium-ion battery recycling method based on defect-targeted healing can fully recover t