Advancing Lithium–Magnesium Separation: Pioneering Swelling-Embedded Cation Exchange Membranes Based on Sulfonated Poly(ether ether ketone)

With the continuous advancement of electrodialysis (ED) technology, there arises a demand for improved monovalent cation exchange membranes (CEMs). However, limitations in membrane materials and structures have resulted in the low selectivity of monovalent CEMs, posing challenges in the separation of Li+ and Mg2+. In this investigation, a designed CEM with a swelling-embedded structure was created by integrating a polyelectrolyte containing N-oxide Zwitterion into a sulfonated poly(ether ether ketone) (SPEEK) membrane, leveraging the notable solubility characteristic of SPEEK. The membranes were prepared by using N-oxide zwitterionic polyethylenimine (ZPEI) and 1,3,5-benzenetrlcarbonyl trichloride (TMC). The as-prepared membranes underwent systematic characterization and testing, evaluating their structural, physicochemical, electrochemical, and selective ED properties. During ED, the modified membranes demonstrated notable permeability selectivity for Li+ ions in binary (Li+/Mg2+) systems. Notably, at a constant current density of 2.5 mA cm–2, the modified membrane PEI-TMC/SPEEK exhibited significant permeability selectivity (PMg2+Li+=5.63) in the Li+/Mg2+ system, while ZPEI-TMC/SPEEK outperformed, displaying remarkable permeability selectivity (PMg2+Li+=12.43) in the Li+/Mg2+ system, surpassing commercial monovalent cation-selective membrane commercial monovalent cation-selective membrane (CIMS). Furthermore, in the Li+/Mg2+ binary system, Li+ flux reached 9.78 × 10–9 mol cm–2 s–1 for ZPEI-TMC/SPEEK, while its Mg2+ flux only reached 2.7 × 10–9 mol cm–2 s–1, showing potential for lithium–magnesium separation. In addition, ZPEI-TMC/SPEEK was tested for performance and stability at high current densities. This work offers a straightforward preparation process and an innovative structural approach, presenting methodological insights for the advancement of lithium and magnesium separation techniques.