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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. In conclusion, correlations are provided for varying porosity, CBD phase interfacial arrangement and solidmore » particle morphology.« less

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1];  [5]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [5];  [6]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Purdue Univ., West Lafayette, IN (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Brigham Young Univ., Provo, UT (United States)
  5. Univ. College London, London (United Kingdom)
  6. Imperial College of London, London (United Kingdom)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (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
Report Number(s):
NREL/JA-5400-71184
Journal ID: ISSN 0013-4651
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article: Published Article
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
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. 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., and Smith, Kandler. Fri . "Resolving the Discrepancy in Tortuosity Factor Estimation for Li-Ion Battery Electrodes through Micro-Macro Modeling and Experiment". United States. doi: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. In conclusion, correlations are provided for varying porosity, CBD phase interfacial arrangement and solid particle morphology.},
doi = {10.1149/2.0731814jes},
journal = {Journal of the Electrochemical Society},
number = 14,
volume = 165,
place = {United States},
year = {Fri Nov 02 00:00:00 EDT 2018},
month = {Fri Nov 02 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1149/2.0731814jes

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Works referenced in this record:

A comprehensive understanding of electrode thickness effects on the electrochemical performances of Li-ion battery cathodes
journal, June 2012


3D Printing of Interdigitated Li-Ion Microbattery Architectures
journal, June 2013

  • Sun, Ke; Wei, Teng-Sing; Ahn, Bok Yeop
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