Impacts of Solvent Washing on the Electrochemical Remediation of Commercial End-Of-Life Cathodes

Changes to the surface structure and chemistry occurring throughout the functional lifetime of lithium-ion batteries (LIBs) may impact the effectiveness of end-of-life rejuvenation methods. Solvent washing prior to electrochemical relithiation is shown to both increase relithiation efficacy and beneficially alter the interfacial chemistry of a heavily degraded industrial cathode material. Four common solvents (acetone, diethyl carbonate, isopropyl alcohol, and propylene carbonate) are employed to investigate the role of varying physicochemical solvent properties on the mechanism of capacity recovery. Electrochemical (dQ/dV, EIS), structural (XRD), and chemical (SPME-GC-MS) analysis techniques are employed to comprehensively analyze solvent–cathode interactions. Highly nucleophilic solvents (acetone, DEC) are found to reduce cathode charge-transfer impedance and enable stable impedance growth throughout subsequent cycling. The use of nucleophilic solvents under mechanically aggressive washing conditions may also enable the reintroduction of bulk lattice oxygen, thereby restoring anionic redox capacity. Further, the four solvents are found to selectively remove a subset of surface species from the aged cathode material, including residual electrolyte, additives, and electrolyte–additive reaction products, which are qualitatively analyzed. Surface species removal by each solvent is correlated with the electrochemical performance of the correspondingly washed cathode, highlighting the importance of an optimized washing protocol for effective remediation in the context of direct LIB recycling. For the material under study, the use of a simple acetone-washing protocol prior to electrochemical relithiation enables up to 174% capacity recovery relative to unwashed/relithiated black mass.