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 h, 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.

Double-photoelectrode redox desalination of seawater.

High energy consumption and low salt removal rate are key barriers to realizing practical electrochemical seawater desalination processes. Here, we demonstrate a novel solar-driven redox flow desalination device with double photoelectrodes to achieve efficient desalination without electrical energy consumption. The device consists of three parts: one photoanode unit, one photocathode unit, and one redox flow desalination unit sandwiched between the two photoelectrode units. The photoelectrode units include a TiO2 photoanode and a NiO photocathode sensitized with N719 dye, triiodide/iodide redox electrolyte, and graphite paper integrated electrodes decorated with 3,4-ethylene-dioxythiophene. Two salt feeds are located between two ferro/ferricyanide redox flow chambers. Under light illumination, high-quality freshwater is obtained from brackish water containing different concentrations of NaCl from 1000 to 12,000 ppm with a high NaCl removal rate. The device can work in multiple desalination cycles without significant performance declines. Furthermore, natural seawater with an ionic conductivity of 53.45 mS cm-1 is desalinated to freshwater. This new design opens opportunities to realize efficient and practical solar-driven desalination processes.