Redox flow batteries hold promise as large-scale energy storage systems for off-grid electrification. The electrolyte is one of the key components of redox batteries. Inspired by the mechanism involved in solvents for extraction, a ternary deep eutectic solvent (DES) is demonstrated, in which glycerol is introduced into the original binary ethaline DES. Redox pairs (active substance) dissolved in the solvent have low charge transfer resistance. The results show that the viscosity of the solvent with the ratio of choline chloride to ethylene glycol to glycerol of 1:2:0.5 decreases from 51.2 mPa·s to 40.3 mPa·s after adding the redox pair, implying that the mass transfer resistance of redox pairs in this solvent is reduced. Subsequent cyclic voltammetry and impedance tests show that the electrochemical performance with the ternary DES as the electrolyte in redox flow batteries is improved. When the ratio of 1:2:0.5 ternary DES is used as the electrolyte, the power density of the battery (9.01 mW·cm⁻²) is 38.2% higher than that of the binary one (6.52 mW·cm⁻²). Fourier transform infrared spectroscopy further indicates that the introduction of glycerol breaks the hydrogen bond network of the solvent environment where the redox pair is located, unraveling the hydrogen bond supramolecular complex. Rational solvent design is an effective strategy to enhance the electrochemical performance of redox batteries.

Redox flow batteries (RFBs) have been widely recognized in the domain of large-scale energy storage due to their simple structure, long lifetime, quick response, decoupling of capacity and power, and structural simplicity. Because of the limited open circuit voltage (OCV) by hydrogen and oxygen evolution reactions, together with the relatively low solubility of active species, RFBs with aqueous electrolytes are challenging to reach high energy densities. Researchers have been trying to develop new solvent systems without water to remove the electrochemical window limitation of water and pursue higher cell potential. However, non-aqueous solvents are also hindered by some key problems, such as high viscosity and poor safety. Meeting these challenges require a comprehensive understanding of relevant structural design parameters and multi-variable operation in the non-aqueous flow battery (NAFB) system. Modeling and simulation are not only an effective way to understand the basic mechanism of flow batteries at different scales of size and time but also an ideal tool for optimizing the reaction process, battery assembly, and the whole flow battery installation. This review paper introduces the development of the non-aqueous flow battery, the challenges it faces, and the research progress of related modeling and simulation for verification or optimization. Finally, the future development prospects of the non-aqueous flow battery model are pointed out, especially for those systems and fields that have not yet been explored.