Integrated assessment of deep eutectic solvents questions solvometallurgy as a sustainable recycling approach for lithium-ion batteries

Critical metals are key to lithium-ion batteries (LIB), but metal mining has inflicted many socio-environmental harms. Recovering metals from spent LIBs can partially overcome this challenge, but existing recovery and recycling techniques such as pyrometallurgy and hydrometallurgy are either energy intensive or require toxic chemicals. Solvometallurgy, using biodegradable deep eutectic solvents (DESs), has emerged as a greener option, but full life cycle sustainability of DESs remains unclear. Here, using an integrated assessment framework we show that, compared with pyrometallurgy and hydrometallurgy, the weak solubility of metal compounds in hydrogen bond donors (HBDs) and acceptors (HBAs) and their non-recoverability in chemical precipitation routes of the DES approach result in 3.1 times more CO2 eq, ∼5 times more ozone depletion, and 6.5–7.3 times higher costs. Although alternative electrodeposition routes can minimize HBA loss and alleviate chemical impacts, high energy consumption associated with HBDs exacerbates global warming potential. In situ repairing/regeneration of crystalline compounds in cathode materials could offer a more sustainable application for DESs.