A biomimetic high-capacity phenazine-based anolyte for aqueous organic redox flow batteries

Aqueous soluble organic (ASO) redox-active materials have recently attracted significant attention as alternatives to traditional transition metal ions in redox flow batteries (RFB). However, reported reversible capacities of ASO are often substantially lower than their theoretical values based on the reported maximum solubilities. Here, we describe a phenazine-based ASO compound with an exceptionally high reversible capacity that exceeds 90% of its theoretical value. By strategically modifying the phenazine molecular structure, we demonstrate an increased solubility from near-zero with pristine phenazine to as much as 1.8 M while also shifting its redox potential by more than 400 mV. An RFB based on a phenazine derivative (7,8-dihydroxyphenazine-2-sulfonic acid) at its near-saturation concentration exhibits an operating voltage of 1.4 V with a reversible anolyte capacity of 67 Ah l−1 and a capacity retention of 99.98% per cycle over 500 cycles. Redox flow batteries (RFBs) based on organic redox-active molecules are attractive, but the solubility of those molecules, and consequently the capacity, is generally low. Here, the authors develop a phenazine derivative with high solubility as an energy-dense anolyte for RFBs.