Recycling cathode materials from spent lithium-ion batteries (LIBs) is critical to a sustainable society as it will relief valuable but scarce recourse crises and reduce environment burdens simultaneously. Different from conventional hydrometallurgical and pyrometallurgical recycling methods, direct regeneration relies on non-destructive cathode-to-cathode mode, and therefore, more time and energy-saving along with an increased economic return and reduced CO2 footprint. This review retrospects the history of direct regeneration and discusses state-of-the-art development. The reported methods, including high-temperature solid-state, hydrothermal/ionothermal, molten salt thermochemistry, and electrochemical method, are comparatively introduced, targeting at illustrating their underlying regeneration mechanism and applicability. Further, representative repairing and upcycling studies on wide-applied cathodes, including LiCoO2 (LCO), ternary oxides, LiFePO4 (LFP), and LiMn2 O4 (LMO), are presented, with an emphasis on milestone cases. Despite these achievements, there remain several critical issues that shall be addressed before the commercialization of the mentioned direct regeneration methods.
Keywords: direct regeneration; methodologies; perspectives; repair; spent lithium-ion battery cathode.
© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.