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Title: Comparing Macroscale and Microscale Simulations of Porous Battery Electrodes

This article describes a vertically-integrated exploration of NMC electrode rate limitations, combining experiments with corresponding macroscale (macro-homogeneous) and microscale models. Parameters common to both models were obtained from experiments or based on published results. Positive electrode tortuosity was the sole fitting parameter used in the macroscale model, while the microscale model used no fitting parameters, instead relying on microstructural domains generated from X-ray microtomography of pristine electrode material held under compression while immersed in electrolyte solution (additionally providing novel observations of electrode wetting). Macroscale simulations showed that the capacity decrease observed at higher rates resulted primarily from solution-phase diffusion resistance. This ability to provide such qualitative insights at low computational costs is a strength of macroscale models, made possible by neglecting electrode spatial details. To explore the consequences of such simplification, the corresponding, computationally-expensive microscale model was constructed. This was found to have limitations preventing quantitatively accurate predictions, for reasons that are discussed in the hope of guiding future work. Nevertheless, the microscale simulation results complement those of the macroscale model by providing a reality-check based on microstructural information; in particular, this novel comparison of the two approaches suggests a reexamination of salt diffusivity measurements.
Authors:
 [1] ;  [1] ; ORCiD logo [2] ;  [1] ;  [3] ;  [1] ;  [4]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Technologies Area
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Engineering Div.
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Physical Sciences and Engineering Directorate
Publication Date:
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 11; Conference: Meeting of the Electrochemical Society, San Diego, CA (United States), 29 May-2 Jun 2016; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE
OSTI Identifier:
1419954
Alternate Identifier(s):
OSTI ID: 1414765

Higa, Kenneth, Wu, Shao-Ling, Parkinson, Dilworth Y., Fu, Yanbao, Ferreira, Steven, Battaglia, Vincent, and Srinivasan, Venkat. Comparing Macroscale and Microscale Simulations of Porous Battery Electrodes. United States: N. p., Web. doi:10.1149/2.0501711jes.
Higa, Kenneth, Wu, Shao-Ling, Parkinson, Dilworth Y., Fu, Yanbao, Ferreira, Steven, Battaglia, Vincent, & Srinivasan, Venkat. Comparing Macroscale and Microscale Simulations of Porous Battery Electrodes. United States. doi:10.1149/2.0501711jes.
Higa, Kenneth, Wu, Shao-Ling, Parkinson, Dilworth Y., Fu, Yanbao, Ferreira, Steven, Battaglia, Vincent, and Srinivasan, Venkat. 2017. "Comparing Macroscale and Microscale Simulations of Porous Battery Electrodes". United States. doi:10.1149/2.0501711jes. https://www.osti.gov/servlets/purl/1419954.
@article{osti_1419954,
title = {Comparing Macroscale and Microscale Simulations of Porous Battery Electrodes},
author = {Higa, Kenneth and Wu, Shao-Ling and Parkinson, Dilworth Y. and Fu, Yanbao and Ferreira, Steven and Battaglia, Vincent and Srinivasan, Venkat},
abstractNote = {This article describes a vertically-integrated exploration of NMC electrode rate limitations, combining experiments with corresponding macroscale (macro-homogeneous) and microscale models. Parameters common to both models were obtained from experiments or based on published results. Positive electrode tortuosity was the sole fitting parameter used in the macroscale model, while the microscale model used no fitting parameters, instead relying on microstructural domains generated from X-ray microtomography of pristine electrode material held under compression while immersed in electrolyte solution (additionally providing novel observations of electrode wetting). Macroscale simulations showed that the capacity decrease observed at higher rates resulted primarily from solution-phase diffusion resistance. This ability to provide such qualitative insights at low computational costs is a strength of macroscale models, made possible by neglecting electrode spatial details. To explore the consequences of such simplification, the corresponding, computationally-expensive microscale model was constructed. This was found to have limitations preventing quantitatively accurate predictions, for reasons that are discussed in the hope of guiding future work. Nevertheless, the microscale simulation results complement those of the macroscale model by providing a reality-check based on microstructural information; in particular, this novel comparison of the two approaches suggests a reexamination of salt diffusivity measurements.},
doi = {10.1149/2.0501711jes},
journal = {Journal of the Electrochemical Society},
number = 11,
volume = 164,
place = {United States},
year = {2017},
month = {6}
}

Works referenced in this record:

Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries
journal, October 2004