A Neutral pH Aqueous Organic–Organometallic Redox Flow Battery with Extremely High Capacity Retention

Abstract

We demonstrate an aqueous organic and organometallic redox flow battery utilizing reactants composed of only earth-abundant elements and operating at neutral pH. The positive electrolyte contains bis((3-trimethylammonio)propyl)ferrocene dichloride, and the negative electrolyte contains bis(3-trimethylammonio)propyl viologen tetrachloride; these are separated by an anion-conducting membrane passing chloride ions. Bis(trimethylammoniopropyl) functionalization leads to ∼2 M solubility for both reactants, suppresses higher-order chemical decomposition pathways, and reduces reactant crossover rates through the membrane. Unprecedented cycling stability was achieved with capacity retention of 99.9943%/cycle and 99.90%/day at a 1.3 M reactant concentration, increasing to 99.9989%/cycle and 99.967%/day at 0.75–1.00 M; these represent the highest capacity retention rates reported to date versus time and versus cycle number. We discuss opportunities for future performance improvement, including chemical modification of a ferrocene center and reducing the membrane resistance without unacceptable increases in reactant crossover. This approach may provide the decadal lifetimes that enable organic–organometallic redox flow batteries to be cost-effective for grid-scale electricity storage, thereby enabling massive penetration of intermittent renewable electricity.