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Title: Substituted thiadiazoles as energy-rich anolytes for nonaqueous redox flow cells

Understanding structure–property relationships is essential for designing energy-rich redox active organic molecules (ROMs) for all-organic redox flow batteries. In this paper we examine thiadiazole ROMs for storage of negative charge in the flow cells. These versatile molecules have excellent solubility and low redox potentials, allowing high energy density to be achieved. By systematically incorporating groups with varying electron accepting/withdrawing ability, we have examined substituent effects on their properties of interest, including redox potentials, calendar lives of charged ROMs in electrolyte, and the flow cell cycling performance. Finally, while the calendar life of energized fluids can be tuned in a predictable fashion over a wide range, the improvements in the calendar life do not automatically translate into the enhanced cycling performance, indicating that in addition to the slow reactions of charged species in the solvent bulk, there are other parasitic reactions that occur only during the electrochemical cycling of the cell and can dramatically affect the cycling lifetime.
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [1] ;  [1] ;  [3] ;  [1] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division. Joint Center for Energy Storage Research
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research; Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research. Materials Science Division
Publication Date:
Grant/Contract Number:
AC02-06CH11357; AC05-76RL01830
Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 6; Journal Issue: 15; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE
OSTI Identifier:
1461448

Huang, Jinhua, Duan, Wentao, Zhang, Jingjing, Shkrob, Ilya A., Assary, Rajeev S., Pan, Baofei, Liao, Chen, Zhang, Zhengcheng, Wei, Xiaoliang, and Zhang, Lu. Substituted thiadiazoles as energy-rich anolytes for nonaqueous redox flow cells. United States: N. p., Web. doi:10.1039/c8ta01059e.
Huang, Jinhua, Duan, Wentao, Zhang, Jingjing, Shkrob, Ilya A., Assary, Rajeev S., Pan, Baofei, Liao, Chen, Zhang, Zhengcheng, Wei, Xiaoliang, & Zhang, Lu. Substituted thiadiazoles as energy-rich anolytes for nonaqueous redox flow cells. United States. doi:10.1039/c8ta01059e.
Huang, Jinhua, Duan, Wentao, Zhang, Jingjing, Shkrob, Ilya A., Assary, Rajeev S., Pan, Baofei, Liao, Chen, Zhang, Zhengcheng, Wei, Xiaoliang, and Zhang, Lu. 2018. "Substituted thiadiazoles as energy-rich anolytes for nonaqueous redox flow cells". United States. doi:10.1039/c8ta01059e.
@article{osti_1461448,
title = {Substituted thiadiazoles as energy-rich anolytes for nonaqueous redox flow cells},
author = {Huang, Jinhua and Duan, Wentao and Zhang, Jingjing and Shkrob, Ilya A. and Assary, Rajeev S. and Pan, Baofei and Liao, Chen and Zhang, Zhengcheng and Wei, Xiaoliang and Zhang, Lu},
abstractNote = {Understanding structure–property relationships is essential for designing energy-rich redox active organic molecules (ROMs) for all-organic redox flow batteries. In this paper we examine thiadiazole ROMs for storage of negative charge in the flow cells. These versatile molecules have excellent solubility and low redox potentials, allowing high energy density to be achieved. By systematically incorporating groups with varying electron accepting/withdrawing ability, we have examined substituent effects on their properties of interest, including redox potentials, calendar lives of charged ROMs in electrolyte, and the flow cell cycling performance. Finally, while the calendar life of energized fluids can be tuned in a predictable fashion over a wide range, the improvements in the calendar life do not automatically translate into the enhanced cycling performance, indicating that in addition to the slow reactions of charged species in the solvent bulk, there are other parasitic reactions that occur only during the electrochemical cycling of the cell and can dramatically affect the cycling lifetime.},
doi = {10.1039/c8ta01059e},
journal = {Journal of Materials Chemistry. A},
number = 15,
volume = 6,
place = {United States},
year = {2018},
month = {3}
}

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