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 Laboratory (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 = {Wed Jan 01 00:00:00 EST 2020},
month = {Wed Jan 01 00:00:00 EST 2020}
}
https://doi.org/10.1149/1945-7111/ab6725
Web of Science
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