Abstract
Aqueous organic redox flow batteries (AORFBs) employing synthetically tailorable organic electroactive compounds have received significant attention for energy storage technologies. There have been many efforts in developing electroactive materials for AORFBs with anion-exchange membranes. On the contrary, electroactive compounds that are compatible with cation-exchange membranes in AORFBs are less studied. Here, we report an electroactive 4-carboxylic-2,2,6,6-tetramethylpiperidin-N-oxyl (4-CO₂Na-TEMPO) molecule for neutral AORFBs. The compound exhibits a good solubility of 1.5 M in an aqueous sodium-based solution, which is 3 times more than that of the pristine 4-hydroxy-2,2,6,6-tetramethylpiperidin-1-oxyl (4-OH-TEMPO). When paired with a 1,10-bis(3-sulfonatopropyl)-4,4′-bipyridinium (SPr)₂V anolyte, the resulting RFB operating through a cation-exchange membrane achieved an open-circuit voltage of 1.19 V and a high energy density of 14.7 W h L–¹. In the long-term cycling study, the RFB features a stable capacity retention of 99.94% per cycle over 400 cycles with nearly 100% Coulombic efficiency.
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