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Modular dimerization of organic radicals for stable and dense flow battery catholyte

Xiu-Liang Lv, Patrick T. Sullivan, Wenjie Li (), Hui-Chun Fu, Ryan Jacobs, Chih-Jung Chen, Dane Morgan, Song Jin and Dawei Feng ()
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Xiu-Liang Lv: University of Wisconsin–Madison
Patrick T. Sullivan: University of Wisconsin–Madison
Wenjie Li: University of Wisconsin–Madison
Hui-Chun Fu: University of Wisconsin–Madison
Ryan Jacobs: University of Wisconsin–Madison
Chih-Jung Chen: University of Wisconsin–Madison
Dane Morgan: University of Wisconsin–Madison
Song Jin: University of Wisconsin–Madison
Dawei Feng: University of Wisconsin–Madison

Nature Energy, 2023, vol. 8, issue 10, 1109-1118

Abstract: Abstract Aqueous organic redox flow batteries (AORFBs) hold promise for safe, sustainable and cost-effective grid energy storage. However, developing catholyte redox molecules with the desired stability, power and energy density remains challenging. In this study, we synthesized a class of ionic liquid-mimicking (2,2,6,6-tetramethylpiperidin-1-yl)oxyl dimers (i-TEMPODs) through a building-block assembly platform. By systematically investigating 21 i-TEMPOD derivatives, we uncovered the optimal size and charge properties that prevent membrane crossover and allow formation of a water-in-salt state. Leveraging these advances, we realized substantial improvements in AORFB performance using the optimum i-TEMPOD catholyte at 2 M concentration. These enhancements encompass several crucial metrics showcased across multiple experiments, including robust cycling stability without apparent capacity decay during 96 days of cycling, facile electrochemical kinetics with a high maximum power density of 0.325 W m−2 and a high full-cell energy density of 47.3 Wh l−1 in a capacity-balanced configuration. These molecular designs pave the way towards low-cost and scalable AORFBs.

Date: 2023
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DOI: 10.1038/s41560-023-01320-w

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