Volume 60, Issue 52 pp. 26971-26977
Research Article

Spatial Structure Regulation: A Rod-Shaped Viologen Enables Long Lifetime in Aqueous Redox Flow Batteries

Hongbin Li

Hongbin Li

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, Xi'an, 710049 China

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Dr. Hao Fan

Corresponding Author

Dr. Hao Fan

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, Xi'an, 710049 China

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Bo Hu

Bo Hu

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, Xi'an, 710049 China

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Linlin Hu

Linlin Hu

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, Xi'an, 710049 China

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Dr. Gang Chang

Dr. Gang Chang

Instrumental Analysis Center of, Xi'an Jiaotong University, Xi'an, 710049 China

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Prof. Dr. Jiangxuan Song

Corresponding Author

Prof. Dr. Jiangxuan Song

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, Xi'an, 710049 China

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First published: 14 October 2021
Citations: 78

Graphical Abstract

We report a rod-like sulfonated viologen (R-Vi) anolyte for aqueous redox flow batteries (AORFBs). R-Vi possesses a low membrane-penetration rate of ≈10−10 cm2 s−1 and the lowest redox potential of −0.55 V vs. SHE among one-electron-storage viologens in AORFBs simultaneously. The R-Vi-based AORFB exhibits an extremely low capacity-fade rate of 0.007 % per cycle in 3200 continuous charging–discharging processes.

Abstract

A stable rod-like sulfonated viologen (R-Vi) derivative is developed through a spatial-structure-adjustment strategy for neutral aqueous organic redox flow batteries (AORFBs). The obtained R-Vi features four individual methyl groups on the 2,2′,6,6′-positions of the 4,4′-bipyridine core ring. The tethered methyls confine the movement of the alkyl chain as well as the sulfonic anion, thus driving the spatial structure from sigmoid to rod shape. The R-Vi with weak charge attraction and large molecular dimension displays an ultralow membrane permeability that is only 14.7 % of that of typical sigmoid viologen. Moreover, the electron-donating effect of methyls endows R-Vi with the lowest redox potential of −0.55 V vs. SHE among one-electron-storage viologen-based AORFBs. The AORFB with the R-Vi anolyte and a K4Fe(CN)6 catholyte exhibits an energy efficiency up to 87 % and extremely low capacity-fade rate of 0.007 % per cycle in 3200 continuous cycles.

Conflict of interest

The authors declare no conflict of interest.

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