Abstract

The use of electrons as main reagent for the recovery and recycling of critical metals from spent lithium-ion batteries (LIBs) is a process electrification strategy that can be used to close the life-cycle loop of LIBs through more sustainable methods. Electrochemical leaching, a process that uses a reductant that is constantly regenerated electrochemically for the leaching of lithium-ion battery black mass (LIBBM), has shown high extraction efficiencies and sustainable scores. However, slow kinetics, reactor design challenges and lack of deeper understanding of the underlying processes are barriers to the optimization, scale-up, and market adoption of this technology. A kinetic study and mathematical model for dissolving LIBBM is presented to better understand the underlying mechanisms aiming to reduce the processing time and make predictions for future design and scale-up. The effect of acid and electrochemically mediated reductant concentrations, LIBBM loading, and cathode/reactor designs were explored. As a result, the leaching time was reduced from 7 h to under 1 h at a pulp density of 73 g/L, without external heating. A novel reactor with parallel baffle electrodes (PBE) was developed, which significantly reduced the leaching time by improving convection in a stirred slurry electrochemical reactor. Dimensionless numbers were deduced from an unsteady state model, which can be used in dimensional analysis for future process design and scale-up.

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