Recyclability study for the next generation of cobalt-free lithium-ion battery systems with C-LNMO, Si/C- LRLO and TiNbO-LNMO active materials via hydrometallurgical route

The scarcity and uncertain supply of cobalt poses significant challenges for the lithium-ion battery industry. To address this issue, alternative chemistries excluding cobalt have been developed. Despite solving supply issues, these developments raise concerns about recyclability and their impact on current recycling trends. This study presents a recycling strategy and evaluates its performance for next-generation cobalt-free lithium-ion batteries. It focuses on three prototypes that use innovative cathode materials (titanium niobium oxide, carbon, and silicon/carbon) and electrolyte systems (ionic liquid and gelified). The proposed recycling process includes pyrolysis, mechanical separation, neutral and acid leaching, cementation, and neutralisation for selective metal separation. The results indicate that gelified electrolytes exhibit greater thermal stability than their liquid counterparts, indicating an effect on the degradation temperature and gas emissions, which are crucial for metal recovery. This study highlights the reduced toxicity of ionic liquid electrolytes and emphasises the need for strict pyrolysis gas handling due to hazardous emissions. High recovery rates (65–90 %) were achieved for nickel, manganese, lithium, and anode components. With potential for process optimisation to improve the quality of products, this study shows that cobalt-free battery systems can be integrated into existing recycling frameworks with adjustments, supporting progress towards sustainable battery practices. • Gelified electrolytes exhibit a higher thermal stability than ionic liquids. • Ionic liquid electrolytes exhibit lower toxicity during pyrolysis. • The CO 2 during pyrolysis is directly proportional to the Li Soluble compounds. • Recycling achieved 65–90 % recovery rates for Ni, Mn, Li, and anode materials. • TNO Cathode material can be selectively recovered via weak sulfuric acid leaching.