Enhancing Sustainability in Lithium-Ion Battery Direct Recycling: Water Electrolysis-induced Gas Separation and Dry Electrode Remanufacturing

Abstract Lithium-ion battery recycling is pivotal for resource conservation and environmental sustainability. Direct recycling, while offering a promising avenue for battery recovery with reduced waste compared to pyrometallurgy and hydrometallurgy, often involves intricate and long processes. This study introduces a novel and energy-efficient water electrolysis-induced gas separation approach, utilizing H2 or O2 microbubbles to efficiently separate electrode materials from current collectors. The process achieves 99.5% material recycling with metal impurities below 40 ppm within 35 seconds for LiFePO4 and 3 seconds for graphite at 10 mA h cm–2, and can be expedited at higher current density, with minimal energy consumption of 11 and 1.1 kJ (kg cell)⁻1. Moreover, this approach accommodates various electrode types, encompassing cathodes, and anodes from spent batteries or manufacturing scraps. Leveraging effective mixing of active materials and conductive agents, the recycled powders are directly refabricated into dry electrodes, showcasing electrochemical performances comparable to commercial counterparts. The elimination of N-methyl pyrrolidone (NMP) usage enhances environmental friendliness. An Everbatt analysis underscores a remarkable reduction in energy consumption and waste generation compared to industrial-adopted recycling methods. This approach is an efficient and sustainable solution for LIB recycling, ensuring environmental responsibility and high-quality materials production.