Kinetic Control over Disproportionation Stabilizes Wurster’s Blue Catholyte for Nonaqueous Redox Flow Batteries

Xiaoting Fang; Zhiguang Li; Lifan Zeng; Heonjae Jeong; Diqing Yue; Lily A. Robertson; Yuyue Zhao; Lei Cheng; Ilya A. Shkrob; Xiaoliang Wei; Lu Zhang

doi:10.1021/acsenergylett.4c02449

Kinetic Control over Disproportionation Stabilizes Wurster’s Blue Catholyte for Nonaqueous Redox Flow Batteries

Xiaoting Fang, Zhiguang Li, Lifan Zeng, Heonjae Jeong, Diqing Yue, Lily A. Robertson, Yuyue Zhao, Lei Cheng, Ilya A. Shkrob, Xiaoliang Wei, Lu Zhang

Research output: Contribution to journal › Article › peer-review

Abstract

Redoxmers are organic molecules that serve as charge carriers in redox flow batteries. While these materials are affordable and easy to source, insufficient stability of their charged states (radical ions) remains a challenge. A common reaction of these species is their disproportionation. This reversible reaction yields unstable multiply charged states, shifting the overall charge transfer equilibrium toward the decomposition products. Here we show how kinetic controls can be engineered into a redoxmer molecule to suppress these unwanted charge transfer reactions. This approach is used to transform Wurster’s blue, which is historically the first example of a stable radical ion in organic chemistry, into an exceptionally durable redoxmer molecule that persists over thousands of electrochemical cycles.

Original language	English
Pages (from-to)	5737-5743
Number of pages	7
Journal	ACS Energy Letters
DOIs	https://doi.org/10.1021/acsenergylett.4c02449
State	Accepted/In press - 2024
Externally published	Yes

Funding

This work was partially supported by the Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. The authors also thank financial support from the U.S. National Science Foundation (Award No. CHE-2055222). The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (\u201CArgonne\u201D). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government.

Funders	Funder number
Basic Energy Sciences
U.S. Department of Energy
Joint Center for Energy Storage Research
Office of Science
National Science Foundation	DE-AC02-06CH11357, CHE-2055222
National Science Foundation

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title = "Kinetic Control over Disproportionation Stabilizes Wurster{\textquoteright}s Blue Catholyte for Nonaqueous Redox Flow Batteries",

abstract = "Redoxmers are organic molecules that serve as charge carriers in redox flow batteries. While these materials are affordable and easy to source, insufficient stability of their charged states (radical ions) remains a challenge. A common reaction of these species is their disproportionation. This reversible reaction yields unstable multiply charged states, shifting the overall charge transfer equilibrium toward the decomposition products. Here we show how kinetic controls can be engineered into a redoxmer molecule to suppress these unwanted charge transfer reactions. This approach is used to transform Wurster{\textquoteright}s blue, which is historically the first example of a stable radical ion in organic chemistry, into an exceptionally durable redoxmer molecule that persists over thousands of electrochemical cycles.",

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year = "2024",

doi = "10.1021/acsenergylett.4c02449",

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journal = "ACS Energy Letters",

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AU - Fang, Xiaoting

AU - Li, Zhiguang

AU - Zeng, Lifan

AU - Jeong, Heonjae

AU - Yue, Diqing

AU - Robertson, Lily A.

AU - Zhao, Yuyue

AU - Cheng, Lei

AU - Shkrob, Ilya A.

AU - Wei, Xiaoliang

AU - Zhang, Lu

PY - 2024

Y1 - 2024

N2 - Redoxmers are organic molecules that serve as charge carriers in redox flow batteries. While these materials are affordable and easy to source, insufficient stability of their charged states (radical ions) remains a challenge. A common reaction of these species is their disproportionation. This reversible reaction yields unstable multiply charged states, shifting the overall charge transfer equilibrium toward the decomposition products. Here we show how kinetic controls can be engineered into a redoxmer molecule to suppress these unwanted charge transfer reactions. This approach is used to transform Wurster’s blue, which is historically the first example of a stable radical ion in organic chemistry, into an exceptionally durable redoxmer molecule that persists over thousands of electrochemical cycles.

AB - Redoxmers are organic molecules that serve as charge carriers in redox flow batteries. While these materials are affordable and easy to source, insufficient stability of their charged states (radical ions) remains a challenge. A common reaction of these species is their disproportionation. This reversible reaction yields unstable multiply charged states, shifting the overall charge transfer equilibrium toward the decomposition products. Here we show how kinetic controls can be engineered into a redoxmer molecule to suppress these unwanted charge transfer reactions. This approach is used to transform Wurster’s blue, which is historically the first example of a stable radical ion in organic chemistry, into an exceptionally durable redoxmer molecule that persists over thousands of electrochemical cycles.

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JO - ACS Energy Letters

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Kinetic Control over Disproportionation Stabilizes Wurster’s Blue Catholyte for Nonaqueous Redox Flow Batteries

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