Redox-Active Eutectic Electrolyte with Viologen and Ferrocene Derivatives for Flow Batteries

ACS Appl Mater Interfaces. 2023 Jan 11;15(1):1148-1156. doi: 10.1021/acsami.2c18546. Epub 2022 Dec 23.

Abstract

Nonflammable eutectic solvents show great potential to enhance the concentrations of the redox-active materials and the cell voltages for redox flow batteries (RFBs). Herein, we report a promising redox-active eutectic electrolyte (1.5 M total redox species) with viologen and ferrocene derivatives where both of the redox reactions are reversible with a maximum open-circuit voltage of 1.35 V and an energy density of 15.1 Wh L-1, which is relevant to large-scale energy storage. The charge-discharge (from 75 to 25% state of charge) characteristics in a flow cell (0.15 M negolyte and 0.3 M posolyte) showed that it can be cycled with consistent discharge capacity for 12 h (19 cycles), beyond which pressure-driven crossover between the posolyte and negolyte reservoirs leads to capacity decay. This study points to promising new directions toward eutectic electrolyte development for RFBs where we demonstrate increasing the polarity, functionalizing the redox molecules, and separating redox intermediates to prevent undesired side reactions can make improvements in operating cell voltage, energy density, and cyclability.

Keywords: 1-1′-ferrocenedimethanol; deep eutectic solvents; energy storage; ionic liquids; methyl viologen dichloride; spectroelectrochemistry.