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Title: Theory of Multicomponent Phenomena in Cation-Exchange Membranes: Part III. Transport in Vanadium Redox-Flow-Battery Separators

Abstract

Transport through vanadium redox-flow-battery membranes strongly influences cell performance. In this work, we use a multicomponent concentrated-solution model of transport and thermodynamics in phase-separated cation-exchange membranes, the most common separator type, to develop structure-performance relationships. The model incorporates species partitioning into the membrane, thermodynamic nonidealities, and Stefan-Maxwell-Onsager frictions between species. Molecular-thermodynamics and -transport theories parameterize the model. We validate the calculations against measured Coulombic and voltage efficiencies of a vanadium flow battery as a function of current density. Our model shows that species transport is the result of collective interactions between all species present in the system. The magnitude of coupling suggests that predictions made using dilute-solution theory for transport in these systems will be misleading in many situations. As a demonstration of the capabilities of the model, we predict cell performance, incorporating these interactions, as a function of electrolyte concentration and composition and membrane equivalent weight and backbone modulus. We find that electrolytes with high sulfuric acid concentrations provide the greatest cell performance (quantified by maximizing power density at a target energy efficiency). In the case of membrane properties, low equivalent-weight polymers perform better; at high equivalent weights, a low membrane modulus is preferred.

Authors:
; ; ; ;
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1598403
Alternate Identifier(s):
OSTI ID: 1713222
Grant/Contract Number:  
AC02-05CH11231; AR0000149; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Journal of the Electrochemical Society (Online)
Additional Journal Information:
Journal Name: Journal of the Electrochemical Society (Online) Journal Volume: 167 Journal Issue: 1; Journal ID: ISSN 1945-7111
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Crothers, Andrew R., Darling, Robert M., Kushner, Douglas I., Perry, Mike L., and Weber, Adam Z. Theory of Multicomponent Phenomena in Cation-Exchange Membranes: Part III. Transport in Vanadium Redox-Flow-Battery Separators. United States: N. p., 2020. Web. doi:10.1149/1945-7111/ab6725.
Crothers, Andrew R., Darling, Robert M., Kushner, Douglas I., Perry, Mike L., & Weber, Adam Z. Theory of Multicomponent Phenomena in Cation-Exchange Membranes: Part III. Transport in Vanadium Redox-Flow-Battery Separators. United States. https://doi.org/10.1149/1945-7111/ab6725
Crothers, Andrew R., Darling, Robert M., Kushner, Douglas I., Perry, Mike L., and Weber, Adam Z. Wed . "Theory of Multicomponent Phenomena in Cation-Exchange Membranes: Part III. Transport in Vanadium Redox-Flow-Battery Separators". United States. https://doi.org/10.1149/1945-7111/ab6725.
@article{osti_1598403,
title = {Theory of Multicomponent Phenomena in Cation-Exchange Membranes: Part III. Transport in Vanadium Redox-Flow-Battery Separators},
author = {Crothers, Andrew R. and Darling, Robert M. and Kushner, Douglas I. and Perry, Mike L. and Weber, Adam Z.},
abstractNote = {Transport through vanadium redox-flow-battery membranes strongly influences cell performance. In this work, we use a multicomponent concentrated-solution model of transport and thermodynamics in phase-separated cation-exchange membranes, the most common separator type, to develop structure-performance relationships. The model incorporates species partitioning into the membrane, thermodynamic nonidealities, and Stefan-Maxwell-Onsager frictions between species. Molecular-thermodynamics and -transport theories parameterize the model. We validate the calculations against measured Coulombic and voltage efficiencies of a vanadium flow battery as a function of current density. Our model shows that species transport is the result of collective interactions between all species present in the system. The magnitude of coupling suggests that predictions made using dilute-solution theory for transport in these systems will be misleading in many situations. As a demonstration of the capabilities of the model, we predict cell performance, incorporating these interactions, as a function of electrolyte concentration and composition and membrane equivalent weight and backbone modulus. We find that electrolytes with high sulfuric acid concentrations provide the greatest cell performance (quantified by maximizing power density at a target energy efficiency). In the case of membrane properties, low equivalent-weight polymers perform better; at high equivalent weights, a low membrane modulus is preferred.},
doi = {10.1149/1945-7111/ab6725},
journal = {Journal of the Electrochemical Society (Online)},
number = 1,
volume = 167,
place = {United States},
year = {2020},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1149/1945-7111/ab6725

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Cited by: 5 works
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