Abstract

Understanding surface charge behavior is essential for improving ion separation during lithium brine treatment. This paper investigates the performance of a three-compartment electrodialysis system designed for the selective removal of divalent cations (Mg2+ and Ca2+). The relationship between zeta potential and the recovery of Li+, Na+, and K+ is analyzed. Zeta potential measurements at various pH values showed that Mg(OH)2 particles maintained a positive charge. The system facilitated the precipitation of Mg(OH)2 and Ca(OH)2 via electrochemically generated OH? ions. The specific electrical energy consumption was evaluated for each operating condition. The results showed that the zeta potential of the precipitates was affected by both the current density and temperature. This influenced lithium losses due to brine entrapment within the precipitated solids. At 600 A/m2 and 50 °C, more than 99% of Mg2+ and Ca2+ were removed, and more than 90% of lithium was recovered, with a specific electric energy consumption of 2.58 kWh per kilogram of Li recovered. The system also generates HCl as a valuable by-product, which improves the sustainability of the process. This study provides a new framework for improving the energy efficiency of lithium purification from brines and lithium recovery. © 2025 by the authors.