Mitigating Ring‐Opening to Develop Stable TEMPO Catholytes for pH‐Neutral All‐Organic Redox Flow Batteries

Redox‐active organics are highly attractive in aqueous organic redox flow batteries (AORFBs). However, the lack of capacity dense, stable organic catholytes remains a challenge to develop energy‐dense, long cycle‐life AORFBs. Herein, a stable organic catholyte, 4‐[3‐(trimethylammonium)acetylamino]‐2...

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Published in:Advanced functional materials 2022-08, Vol.32 (33), p.n/a
Main Authors: Fan, Hao, Wu, Wenda, Ravivarma, Mahalingam, Li, Hongbin, Hu, Bo, Lei, Jiafeng, Feng, Yangyang, Sun, Xiaohua, Song, Jiangxuan, Liu, Tianbiao Leo
Format: Article
Language:English
Subjects:
Anolytes
Catholytes
energy storage
Materials science
nitroxyl radicals
organic catholytes
Rechargeable batteries
redox flow batteries
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Summary:Redox‐active organics are highly attractive in aqueous organic redox flow batteries (AORFBs). However, the lack of capacity dense, stable organic catholytes remains a challenge to develop energy‐dense, long cycle‐life AORFBs. Herein, a stable organic catholyte, 4‐[3‐(trimethylammonium)acetylamino]‐2,2,6,6‐tetramethylpiperidine‐1‐oxyl chloride (TMAAcNHTEMPO) is developed through rational molecular engineering using connective acetamido and trimethylammonium groups. Paired with bis‐(trimethylammonium) propyl viologen tetrachloride anolyte, stable AORFBs (up to 1500 cycles) with a low capacity fade rate of ca. 0.0144% h−1 are achieved. Experimental characterizations and theoretical simulations revealed that TMAAcNH‐TEMPO is largely stabilized by the reduced reactivity of the nitroxyl radical moiety that mitigates a ring‐opening side reaction. A new TEMPO molecule is developed through rational molecular engineering as a stable, capacity density organic catholyte for total organic flow batteries.
ISSN:1616-301X
1616-3028
DOI:10.1002/adfm.202203032