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Title: Resolving the Discrepancy in Tortuosity Factor Estimation for Li-Ion Battery Electrodes through Micro-Macro Modeling and Experiment

Abstract

Battery performance is strongly correlated with electrode microstructural properties. Of the relevant properties, the tortuosity factor of the electrolyte transport paths through microstructure pores is important as it limits battery maximum charge/discharge rate, particularly for energy-dense thick electrodes. Tortuosity factor however, is difficult to precisely measure, and thus its estimation has been debated frequently in the literature. Herein, three independent approaches have been applied to quantify the tortuosity factor of lithium-ion battery electrodes. The first approach is a microstructure model based on three-dimensional geometries from X-ray computed tomography (CT) and stochastic reconstructions enhanced with computationally generated carbon/binder domain (CBD), as CT is often unable to resolve the CBD. The second approach uses a macro-homogeneous model to fit electrochemical data at several rates, providing a separate estimation of the tortuosity factor. The third approach experimentally measures tortuosity factor via symmetric cells employing a blocking electrolyte. Comparisons have been made across the three approaches for 14 graphite and nickel-manganese-cobalt oxide electrodes. Analysis suggests that if the tortuosity factor were characterized based on the active material skeleton only, the actual tortuosities would be 1.35-1.81 times higher for calendered electrodes. Correlations are provided for varying porosity, CBD phase interfacial arrangement and solid particle morphology.more » (C) The Author(s) 2018. Published by ECS.« less

Authors:
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Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1480558
Alternate Identifier(s):
OSTI ID: 1482500; OSTI ID: 1558106
Report Number(s):
NREL/JA-5400-71184
Journal ID: ISSN 0013-4651; /jes/165/14/A3403.atom
Grant/Contract Number:  
AC36-08GO28308; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Name: Journal of the Electrochemical Society Journal Volume: 165 Journal Issue: 14; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 30 DIRECT ENERGY CONVERSION; lithium-ion battery; electrode tortuosity; nickel-cobalt-manganese; graphite; microstructure model; stochastic microstructure; macro homogeneous model; carbon/binder domain arrangement; calendaring

Citation Formats

Usseglio-Viretta, Francois L. E., Colclasure, Andrew, Mistry, Aashutosh N., Claver, Koffi Pierre Yao, Pouraghajan, Fezzeh, Finegan, Donal P., Heenan, Thomas M. M., Abraham, Daniel, Mukherjee, Partha P., Wheeler, Dean, Shearing, Paul, Cooper, Samuel J., and Smith, Kandler. Resolving the Discrepancy in Tortuosity Factor Estimation for Li-Ion Battery Electrodes through Micro-Macro Modeling and Experiment. United States: N. p., 2018. Web. doi:10.1149/2.0731814jes.
Usseglio-Viretta, Francois L. E., Colclasure, Andrew, Mistry, Aashutosh N., Claver, Koffi Pierre Yao, Pouraghajan, Fezzeh, Finegan, Donal P., Heenan, Thomas M. M., Abraham, Daniel, Mukherjee, Partha P., Wheeler, Dean, Shearing, Paul, Cooper, Samuel J., & Smith, Kandler. Resolving the Discrepancy in Tortuosity Factor Estimation for Li-Ion Battery Electrodes through Micro-Macro Modeling and Experiment. United States. https://doi.org/10.1149/2.0731814jes
Usseglio-Viretta, Francois L. E., Colclasure, Andrew, Mistry, Aashutosh N., Claver, Koffi Pierre Yao, Pouraghajan, Fezzeh, Finegan, Donal P., Heenan, Thomas M. M., Abraham, Daniel, Mukherjee, Partha P., Wheeler, Dean, Shearing, Paul, Cooper, Samuel J., and Smith, Kandler. Mon . "Resolving the Discrepancy in Tortuosity Factor Estimation for Li-Ion Battery Electrodes through Micro-Macro Modeling and Experiment". United States. https://doi.org/10.1149/2.0731814jes.
@article{osti_1480558,
title = {Resolving the Discrepancy in Tortuosity Factor Estimation for Li-Ion Battery Electrodes through Micro-Macro Modeling and Experiment},
author = {Usseglio-Viretta, Francois L. E. and Colclasure, Andrew and Mistry, Aashutosh N. and Claver, Koffi Pierre Yao and Pouraghajan, Fezzeh and Finegan, Donal P. and Heenan, Thomas M. M. and Abraham, Daniel and Mukherjee, Partha P. and Wheeler, Dean and Shearing, Paul and Cooper, Samuel J. and Smith, Kandler},
abstractNote = {Battery performance is strongly correlated with electrode microstructural properties. Of the relevant properties, the tortuosity factor of the electrolyte transport paths through microstructure pores is important as it limits battery maximum charge/discharge rate, particularly for energy-dense thick electrodes. Tortuosity factor however, is difficult to precisely measure, and thus its estimation has been debated frequently in the literature. Herein, three independent approaches have been applied to quantify the tortuosity factor of lithium-ion battery electrodes. The first approach is a microstructure model based on three-dimensional geometries from X-ray computed tomography (CT) and stochastic reconstructions enhanced with computationally generated carbon/binder domain (CBD), as CT is often unable to resolve the CBD. The second approach uses a macro-homogeneous model to fit electrochemical data at several rates, providing a separate estimation of the tortuosity factor. The third approach experimentally measures tortuosity factor via symmetric cells employing a blocking electrolyte. Comparisons have been made across the three approaches for 14 graphite and nickel-manganese-cobalt oxide electrodes. Analysis suggests that if the tortuosity factor were characterized based on the active material skeleton only, the actual tortuosities would be 1.35-1.81 times higher for calendered electrodes. Correlations are provided for varying porosity, CBD phase interfacial arrangement and solid particle morphology. (C) The Author(s) 2018. Published by ECS.},
doi = {10.1149/2.0731814jes},
journal = {Journal of the Electrochemical Society},
number = 14,
volume = 165,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2018},
month = {Mon Jan 01 00:00:00 EST 2018}
}

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