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Title: Solution Properties and Practical Limits of Concentrated Electrolytes for Nonaqueous Redox Flow Batteries

Abstract

Nonaqueous redox flow batteries (NRFBs) use energized organic fluids that contain redox active organic molecules (ROMs) and supporting electrolyte. Such all-organic electrolytes have wider electrochemical stability windows than the more familiar aqueous electrolytes, potentially allowing a higher energy density in the solutions of charged ROMs. As this energy density increases linearly with the concentration of the charge carriers, physicochemical properties of concentrated ROM solutions in both states of charge present considerable practical interest. For NRFBs to become competitive with other types of flow cells, the current techno-economic analyses favor highly concentrated solutions (>1 M) with high ionic conductivity (>5 mS/cm). It is not presently clear that such solutions can have the required dynamic properties. In this paper, we show that ion diffusivities and conductivities of ROM-containing electrolytes reach maxima around 0.5 M and decrease significantly at higher concentrations; realistic limits are established for variations of these parameters. Furthermore, using closed-shell analogues for open-shell charged ROMs, we show that reconstitution of highly concentrated fluids during electrochemical charging will have strong adverse effects on their properties, including an increase in viscosity and decrease in conductivity and ion diffusivity. Finally, given our results, it appears that the target concentrations of NRFB fluids needmore » to be reconsidered in terms of concentration-dependent conductivity and viscosity.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research. Chemical Sciences and Engineering Division
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research; Univ. of Illinois, Urbana, IL (United States). Dept. of Mechanical Science and Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1461454
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 15; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Zhang, Jingjing, Corman, R. E., Schuh, Jonathon K., Ewoldt, Randy H., Shkrob, Ilya A., and Zhang, Lu. Solution Properties and Practical Limits of Concentrated Electrolytes for Nonaqueous Redox Flow Batteries. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b02009.
Zhang, Jingjing, Corman, R. E., Schuh, Jonathon K., Ewoldt, Randy H., Shkrob, Ilya A., & Zhang, Lu. Solution Properties and Practical Limits of Concentrated Electrolytes for Nonaqueous Redox Flow Batteries. United States. doi:10.1021/acs.jpcc.8b02009.
Zhang, Jingjing, Corman, R. E., Schuh, Jonathon K., Ewoldt, Randy H., Shkrob, Ilya A., and Zhang, Lu. Thu . "Solution Properties and Practical Limits of Concentrated Electrolytes for Nonaqueous Redox Flow Batteries". United States. doi:10.1021/acs.jpcc.8b02009. https://www.osti.gov/servlets/purl/1461454.
@article{osti_1461454,
title = {Solution Properties and Practical Limits of Concentrated Electrolytes for Nonaqueous Redox Flow Batteries},
author = {Zhang, Jingjing and Corman, R. E. and Schuh, Jonathon K. and Ewoldt, Randy H. and Shkrob, Ilya A. and Zhang, Lu},
abstractNote = {Nonaqueous redox flow batteries (NRFBs) use energized organic fluids that contain redox active organic molecules (ROMs) and supporting electrolyte. Such all-organic electrolytes have wider electrochemical stability windows than the more familiar aqueous electrolytes, potentially allowing a higher energy density in the solutions of charged ROMs. As this energy density increases linearly with the concentration of the charge carriers, physicochemical properties of concentrated ROM solutions in both states of charge present considerable practical interest. For NRFBs to become competitive with other types of flow cells, the current techno-economic analyses favor highly concentrated solutions (>1 M) with high ionic conductivity (>5 mS/cm). It is not presently clear that such solutions can have the required dynamic properties. In this paper, we show that ion diffusivities and conductivities of ROM-containing electrolytes reach maxima around 0.5 M and decrease significantly at higher concentrations; realistic limits are established for variations of these parameters. Furthermore, using closed-shell analogues for open-shell charged ROMs, we show that reconstitution of highly concentrated fluids during electrochemical charging will have strong adverse effects on their properties, including an increase in viscosity and decrease in conductivity and ion diffusivity. Finally, given our results, it appears that the target concentrations of NRFB fluids need to be reconsidered in terms of concentration-dependent conductivity and viscosity.},
doi = {10.1021/acs.jpcc.8b02009},
journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = 15,
volume = 122,
place = {United States},
year = {2018},
month = {4}
}

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