Modeling the Mesoscale Transport of Lithium-Magnetite Electrodes Using Insight from Discharge and Voltage Recovery Experiments
Abstract
A multi-scale mathematical model, which accounts for mass transport on the crystal and agglomerate length-scales, is used to investigate the electrochemical performance of lithium-magnetite electrochemical cells. Experimental discharge and voltage recovery data are compared to three sets of simulations, which incorporate crystal-only, agglomerate-only, or multi-scale transport effects. Mass transport diffusion coefficients are determined by fitting the simulated voltage recovery times to experimental data. In addition, a further extension of the multi-scale model is proposed which accounts for the impact of agglomerate size distributions on electrochemical performance. The results of the study indicate that, depending on the crystal size, the low utilization of the active material is caused by transport limitations on the agglomerate and/or crystal length-scales. For electrodes composed of small crystals (6 and 8 nm diameters), it is concluded that the transport limitations in the agglomerate are primarily responsible for the long voltage recovery times and low utilization of the active mass. In the electrodes composed of large crystals (32 nm diameter), the slow voltage recovery is attributed to transport limitations on both the agglomerate and crystal length-scales.
- Authors:
-
- Columbia Univ., New York, NY (United States)
- Stony Brook Univ., NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2M)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1370757
- Grant/Contract Number:
- SC0012673; DGE-11-44155; C090171
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the Electrochemical Society
- Additional Journal Information:
- Journal Volume: 162; Journal Issue: 14; Related Information: m2M partners with Stony Brook University (lead); Brookhaven National Laboratory; Columbia University; Georgia Institute of Technology; Oak Ridge National Laboratory; Rensselaer Polytechnic Institute; University of California, Berkeley; University of North Carolina at Chapel Hill; Journal ID: ISSN 0013-4651
- Publisher:
- The Electrochemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; energy storage (including batteries and capacitors); charge transport; mesostructured materials
Citation Formats
Knehr, K. W., Brady, Nicholas W., Cama, Christina A., Bock, David C., Lin, Zhou, Lininger, Christianna N., Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., and West, Alan C. Modeling the Mesoscale Transport of Lithium-Magnetite Electrodes Using Insight from Discharge and Voltage Recovery Experiments. United States: N. p., 2015.
Web. doi:10.1149/2.0961514jes.
Knehr, K. W., Brady, Nicholas W., Cama, Christina A., Bock, David C., Lin, Zhou, Lininger, Christianna N., Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., & West, Alan C. Modeling the Mesoscale Transport of Lithium-Magnetite Electrodes Using Insight from Discharge and Voltage Recovery Experiments. United States. https://doi.org/10.1149/2.0961514jes
Knehr, K. W., Brady, Nicholas W., Cama, Christina A., Bock, David C., Lin, Zhou, Lininger, Christianna N., Marschilok, Amy C., Takeuchi, Kenneth J., Takeuchi, Esther S., and West, Alan C. Tue .
"Modeling the Mesoscale Transport of Lithium-Magnetite Electrodes Using Insight from Discharge and Voltage Recovery Experiments". United States. https://doi.org/10.1149/2.0961514jes. https://www.osti.gov/servlets/purl/1370757.
@article{osti_1370757,
title = {Modeling the Mesoscale Transport of Lithium-Magnetite Electrodes Using Insight from Discharge and Voltage Recovery Experiments},
author = {Knehr, K. W. and Brady, Nicholas W. and Cama, Christina A. and Bock, David C. and Lin, Zhou and Lininger, Christianna N. and Marschilok, Amy C. and Takeuchi, Kenneth J. and Takeuchi, Esther S. and West, Alan C.},
abstractNote = {A multi-scale mathematical model, which accounts for mass transport on the crystal and agglomerate length-scales, is used to investigate the electrochemical performance of lithium-magnetite electrochemical cells. Experimental discharge and voltage recovery data are compared to three sets of simulations, which incorporate crystal-only, agglomerate-only, or multi-scale transport effects. Mass transport diffusion coefficients are determined by fitting the simulated voltage recovery times to experimental data. In addition, a further extension of the multi-scale model is proposed which accounts for the impact of agglomerate size distributions on electrochemical performance. The results of the study indicate that, depending on the crystal size, the low utilization of the active material is caused by transport limitations on the agglomerate and/or crystal length-scales. For electrodes composed of small crystals (6 and 8 nm diameters), it is concluded that the transport limitations in the agglomerate are primarily responsible for the long voltage recovery times and low utilization of the active mass. In the electrodes composed of large crystals (32 nm diameter), the slow voltage recovery is attributed to transport limitations on both the agglomerate and crystal length-scales.},
doi = {10.1149/2.0961514jes},
journal = {Journal of the Electrochemical Society},
number = 14,
volume = 162,
place = {United States},
year = {Tue Oct 27 00:00:00 EDT 2015},
month = {Tue Oct 27 00:00:00 EDT 2015}
}
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