Impact of Pore Tortuosity on Electrode Kinetics in Lithium Battery Electrodes: Study in Directionally Freeze-Cast LiNi 0.8 Co 0.15 Al 0.05 O 2 (NCA)
Abstract
The prevailing electrode fabrication method for lithium-ion battery electrodes includes calendering at high pressures to densify the electrode and promote adhesion to the metal current collector. However, this process increases the tortuosity of the pore network in the primary transport direction and imposes severe tradeoffs between electrode thickness and rate capability. With the aim of understanding the impact of pore tortuosity on electrode kinetics, and enabling cell designs with thicker electrodes and improved cost and energy density, we use here freeze-casting, a shaping technique able to produce low-tortuosity structures using ice crystals as a pore-forming agent, to fabricate LiNi0.8Co0.15Al0.05O2 (NCA) cathodes with controlled, aligned porosity. Electrode tortuosity is characterized using two complementary methods, X-ray tomography combined with thermal diffusion simulations, and electrochemical transport measurements. The results allow comparison across a wide range of microstructures, and highlight the large impact of a relatively small numerical change in tortuosity on electrode kinetics. Under galvanostatic discharge, optimized microstructures show a three- to fourfold increase in area-specific capacity compared to typical Li-ion composite electrodes. Hybrid pulse power characterization (HPPC) demonstrates improved power capability, while dynamic stress tests (DST) shows that an area-specific area capacity corresponding to 91% of the NCA galvanostatic C/10 capacity couldmore »
- Authors:
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES); Belgian Science Policy Office; Région Wallone (Belgium); Wallonie-Bruxelles International (Belgium); National Fund for Scientific Research (FNRS) (Belgium)
- OSTI Identifier:
- 1419826
- Alternate Identifier(s):
- OSTI ID: 1494080
- Grant/Contract Number:
- AC02-05CH11231
- 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: 2; Journal ID: ISSN 0013-4651
- Publisher:
- The Electrochemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; freeze-casting; lithium-ion; tortuosity
Citation Formats
Delattre, Benjamin, Amin, Ruhul, Sander, Jonathan, De Coninck, Joël, Tomsia, Antoni P., and Chiang, Yet-Ming. Impact of Pore Tortuosity on Electrode Kinetics in Lithium Battery Electrodes: Study in Directionally Freeze-Cast LiNi 0.8 Co 0.15 Al 0.05 O 2 (NCA). United States: N. p., 2018.
Web. doi:10.1149/2.1321802jes.
Delattre, Benjamin, Amin, Ruhul, Sander, Jonathan, De Coninck, Joël, Tomsia, Antoni P., & Chiang, Yet-Ming. Impact of Pore Tortuosity on Electrode Kinetics in Lithium Battery Electrodes: Study in Directionally Freeze-Cast LiNi 0.8 Co 0.15 Al 0.05 O 2 (NCA). United States. https://doi.org/10.1149/2.1321802jes
Delattre, Benjamin, Amin, Ruhul, Sander, Jonathan, De Coninck, Joël, Tomsia, Antoni P., and Chiang, Yet-Ming. Thu .
"Impact of Pore Tortuosity on Electrode Kinetics in Lithium Battery Electrodes: Study in Directionally Freeze-Cast LiNi 0.8 Co 0.15 Al 0.05 O 2 (NCA)". United States. https://doi.org/10.1149/2.1321802jes.
@article{osti_1419826,
title = {Impact of Pore Tortuosity on Electrode Kinetics in Lithium Battery Electrodes: Study in Directionally Freeze-Cast LiNi 0.8 Co 0.15 Al 0.05 O 2 (NCA)},
author = {Delattre, Benjamin and Amin, Ruhul and Sander, Jonathan and De Coninck, Joël and Tomsia, Antoni P. and Chiang, Yet-Ming},
abstractNote = {The prevailing electrode fabrication method for lithium-ion battery electrodes includes calendering at high pressures to densify the electrode and promote adhesion to the metal current collector. However, this process increases the tortuosity of the pore network in the primary transport direction and imposes severe tradeoffs between electrode thickness and rate capability. With the aim of understanding the impact of pore tortuosity on electrode kinetics, and enabling cell designs with thicker electrodes and improved cost and energy density, we use here freeze-casting, a shaping technique able to produce low-tortuosity structures using ice crystals as a pore-forming agent, to fabricate LiNi0.8Co0.15Al0.05O2 (NCA) cathodes with controlled, aligned porosity. Electrode tortuosity is characterized using two complementary methods, X-ray tomography combined with thermal diffusion simulations, and electrochemical transport measurements. The results allow comparison across a wide range of microstructures, and highlight the large impact of a relatively small numerical change in tortuosity on electrode kinetics. Under galvanostatic discharge, optimized microstructures show a three- to fourfold increase in area-specific capacity compared to typical Li-ion composite electrodes. Hybrid pulse power characterization (HPPC) demonstrates improved power capability, while dynamic stress tests (DST) shows that an area-specific area capacity corresponding to 91% of the NCA galvanostatic C/10 capacity could be reached.},
doi = {10.1149/2.1321802jes},
journal = {Journal of the Electrochemical Society},
number = 2,
volume = 165,
place = {United States},
year = {2018},
month = {1}
}
https://doi.org/10.1149/2.1321802jes
Web of Science
Figures / Tables:

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