Coupling redox flow desalination with lithium recovery from spent lithium-ion batteries

Electrochemical redox flow desalination is an emerging method to obtain freshwater; however, the costly requirement for continuously supplying and regenerating redox species limits their practical applications. Recycling of spent lithium-ion batteries is a growing challenge for their sustainable utilization. Existing battery recycling methods often involve massive secondary pollution. Here, we demonstrate a redox flow system to couple redox flow desalination with lithium recovery from spent lithium-ion batteries. The spontaneous reaction between a battery cathode material (LiFePO4) and ferricyanide enables the continuous regeneration of the redox species required for desalination. Several critical operating parameters are optimized, including current density, the concentrations of redox species, salt concentrations of brine, and the amounts of added LiFePO4. With the addition of 0.5920 g of spent LiFePO4 in five consecutive batches, the system can operate over 24 hours, achieving 70.46% lithium recovery in the form of LiCl aqueous solution at the concentration of 6.716 g·L−1. Simultaneously, the brine (25 mL, 10000 ppm NaCl) was desalinated to freshwater. Detailed cost analysis shows that this redox flow system could generate a revenue of ¥ 13.66 per kg of processed spent lithium-ion batteries with low energy consumption (0.77 MJ kg−1) and few greenhouse gas emissions indicating excellent economic and environmental benefits over existing lithium-ion battery recycling technologies, such as pyrometallurgical and hydrometallurgical methods. This work opens a new approach to holistically addressing water and energy challenges to achieve sustainable development.