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:

Zhang, Jingjing  ^[1];

• Search DOE PAGES for author "Zhang, Jingjing"
• Search DOE PAGES for ORCID "0000-0003-4768-2312"

Corman, R. E.  ^[2];

• Search DOE PAGES for author "Corman, R. E."
• Search DOE PAGES for ORCID "0000-0001-6818-7674"

Schuh, Jonathon K.  ^[2];

• Search DOE PAGES for author "Schuh, Jonathon K."
• Search DOE PAGES for ORCID "0000-0001-6390-5972"

Ewoldt, Randy H.  ^[2];

• Search DOE PAGES for author "Ewoldt, Randy H."
• Search DOE PAGES for ORCID "0000-0003-2720-9712"

Shkrob, Ilya A.  ^[1];

• Search DOE PAGES for author "Shkrob, Ilya A."
• Search DOE PAGES for ORCID "0000-0002-8851-8220"

Zhang, Lu  ^[1]

• Search DOE PAGES for author "Zhang, Lu"
• Search DOE PAGES for ORCID "0000-0003-0367-0862"

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+ Show Author Affiliations

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:

Thu Apr 05 00:00:00 EDT 2018

Research Org.:

Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1461454

Grant/Contract Number:  

AC02-06CH11357

Resource Type:

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