Shifting the Redox-Flow Battery Trade-Off with Amine-Crosslinked PVBC Thin-Film Composite Membranes

Redox flow batteries (RFBs) are an interesting option for long-term energy storage. A well-performing membrane sits at the heart of the electrochemical battery cell and should effectively mitigate crossover of active species while minimizing resistance. However, current commercial membranes are rather expensive and demonstrate sub-optimal performance, leading to an extensive search for alternatives. Research on membranes for RFBs has long been dominated by dense ion-exchange membranes and porous membranes, both potentially with fillers. In recent years, increased interest in alternative morphologies such as thin-film composites (TFCs) has ignited new research directions. TFCs consist of a thin dense layer on top of a porous support, aiming to merge the advantages of both. Traditionally, TFCs are made using polyamide top layers. In this paper, a novel chemistry is developed with increased chemical stability for RFBs. Poly(vinylbenzyl chloride) is crosslinked interfacially with a diamine, demonstrating for the first time the potential of support-mediated interfacial crosslinking with two immiscible solvents. Optimization of the support, amine crosslinker, reaction time and synthesis procedure allowed a shift of the trade-off between vanadium crossover and proton transport, highlighting the opportunities for this promising TFC chemistry.