Redox flow batteries (RFBs) are promising devices for grid energy storage, but additional cost reductions are needed to meet the U.S. Department of Energy recommended capital cost of $150 kWh −1 for an installed system. The development of new active species designed to lower cost or improve performance is a promising approach, but these new materials often require compatible electrolytes that optimize stability, solubility, and reaction kinetics. This work quantifies changes in RFB cost performance for different aqueous supporting electrolytes paired with different types of membranes. A techno-economic model is also used to estimate RFB-system costs for the different membrane and supporting salt options considered herein. Beyond the conventional RFB design incorporating small active species and an ion-exchange membrane (IEM), this work also considers size-selective separators as a cost-effective alternative to IEMs. The size selective separator (SSS) concept utilizes nanoporous separators with no functionalization for ion selectivity, and the active species are large enough that they cannot pass through the separator pores. Our analysis finds that SSS or H + -IEM are most promising to achieve cost targets for aqueous RFBs, and supporting electrolyte selection yields cost differences in the $100's kWh Energy storage has emerged as a key technology for improving the sustainability of electricity generation 1 by improving the efficiency of existing fossil-fuel infrastructure through load-leveling or price arbitrage, 2 alleviating the intermittency of renewables (i.e., solar, wind) to promote their broad implementation, 3 and providing high-value services such as frequency regulation, voltage support, or back-up power.2 Redox flow batteries (RFBs) are promising devices for low-cost grid energy storage due to decoupled capacity and power scaling, long operational lifetime, easy thermal management, and good safety features.2,4-9 Unlike enclosed batteries (i.e., lithium-ion, nickel-metal hydride), RFBs implement soluble redox active species dissolved in liquid electrolytes, which are stored in large, inexpensive tanks. Specifically, the electrolyte is comprised of a supporting electrolyte, which contains solvent (e.g., water) and a supporting salt (e.g., sulfuric acid, sodium chloride), and the redox active species (e.g., bromine). The electrolyte is pumped through an electrochemical stack where the active species are oxidized or reduced to charge or discharge the battery. The size of the electrochemical stack determines the power rating, while the tank volume determines the energy capacity, enabling scalability unique to the RFB architecture. The introduction of new redox chemistries is a strategy for substantially lowering the electrolyte (energy) cost contribution to the total battery cost via decreased chemical costs or increased electrolyte energy density. 23,26 Key active species characteristics in determining the RFB electrolyte cost are the solubility (M), molar mass (kg mol −1 ), number of electrons stored pe...