To further investigate the Li-ion transport properties of the candidate membranes, Li PFG solid-state NMR was carried out for the as-prepared membranes (dry) as well as for membranes swollen in 0.1 M LiCl aqueous solution (Figure ). Li-ion diffusion coefficients for the as-prepared membranes are in the 10 -12 m 2 s -1 range, which is nearly one order of magnitude lower than reported previously for the LiMTFSI nanoparticles with propylene carbonate as a plasticiser. This difference arises from the absence of plasticiser in the membrane matrix, such as the propylene carbonate employed in reference works, that can improve the mobility of diffusing ions and polymeric chains in the polymer. The styrene-containing membrane shows a higher diffusion coefficient by half an order of magnitude than in the case of the methacrylate material, which can be explained by the absence of highly coordinating ether oxygen moieties as in the case of the methacrylate material with the ether group in close proximity to the TFSI anion. Upon swelling of the membranes in 0.1 M LiCl for 24 h, the Li-ion diffusion coefficient increases two orders of magnitude to reach values up to 10 -10 m 2 s -1 , in line with those of the benchmark Nafion TM 117 membrane. The aqueous solution provides additional faster diffusion pathways which can contribute to and dominate the transport mechanism in the membranes, hence the lower difference between the different compositions. To assess the suitability of the three LiTFSI-based candidate polymeric membranes for Li-salt electrodialysis as CEMs, synthetic Li2SO4 leachates were processed into high-value LiOH and sulfuric acid using a 2-compartment H-cell setup as represented in Figure . Water splitting generates H + that regenerates H2SO4 in the anolyte (Li2SO4 leachate compartment) which can be circled back to the liquor leaching process. In the cathode compartment, water splitting results in OH -generation that is used to produce LiOH in the catholyte (receiving LiOH compartment) with the beneficial production of green-H2 gas as a byproduct.