Comparison of Separators vs Membranes in Nonaqueous Redox Flow Battery Electrolytes Containing Small Molecule Active Materials

The lack of suitable membranes for nonaqueous electrolytes limits cell capacity and cycle lifetime in organic redox flow cells. Using soluble, stable materials, we sought to compare the best performance that could be achieved with commercially available microporous separators and ion-selective membranes. We use organic species with proven stability to avoid deconvoluting capacity fade due to crossover and/or cell imbalance from materials degradation. We found a trade-off between lifetime and coulombic efficiency: non-selective separators achieve more stable performance but suffer from low coulombic efficiencies, while ion-selective membranes achieve high coulombic efficiencies but experience capacity loss over time. When electrolytes are pre-mixed prior to cycling, coulombic efficiency remains high, but capacity is lost due to cell imbalance, which can be recovered by electrolyte rebalancing. The results of this study highlight the potential for gains in nonaqueous cell performance that may be enabled by suitable membranes.