Direct recycling of spent cathode material at ambient conditions via spontaneous lithiation

Direct recycling is a promising route for the sustainable management of end-of-life spent cathodes. However, its practical implementation is greatly restricted as most existing methods require heating or high-pressure conditions during the lithiation step to overcome the thermodynamic obstacles and realize lithium replenishment. In this study, we explored a strategy to realize spontaneous lithiation via simple solid–liquid mixing at ambient conditions. The thermodynamic barrier of the lithiation reaction was reduced by self-adsorbed amyloxylithium, which can spontaneously adsorb on the surface of degraded cathode particles without an external driving force. This strategy can regenerate both laboratory-dismantled LiNi0.6Co0.2Mn0.2O2 from 10 Ah pouch cells and industrial-dismantled LiNi0.5Co0.2Mn0.3O2 black mass. The capacity retention rate of a 1 Ah pouch cell assembled using regenerated LiNi0.5Co0.2Mn0.3O2 as cathode material was 80.5% after 500 cycles. The proposed strategy has big economic advantages over conventional pyro- and hydrometallurgical methods, as evidenced by the techno-economic analysis, accompanied by obvious environmental benefits, as evidenced by reduced CO2 emissions. This work provides a viable approach for the direct recycling of spent cathode material, improving the circularity of the battery industry. Direct recycling can facilitate the sustainable management of end-of-life spent cathodes, but is hindered by the harsh operation conditions required. An spontaneous lithiation strategy enables direct recycling of spent cathode material at ambient conditions, with clear economic and environmental benefits.