High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation
Abstract
High-voltage Ni-rich cathodes have been studied as a possible way to achieve high energy density in Li-ion batteries. However, capacity fade due to structural changes at high voltages has limited their applications. In this study, we identify 4.5 V (vs. graphite) as the optimum upper cutoff voltage (UCV) for a Ni-rich NCA cathode [LiNi0.8Co0.15Al0.05O2]. At this UCV, NCA delivers a 12 % increase in reversible capacity (when discharged to 2.5 V) and retains 92 % of its initial capacity after 100 cycles at 1C/-1C cycling when compared to 4.2 V as UCV. By increasing UCV to 4.7 V, the discharge capacity can be raised to >200 mAh/g. However, the rate of capacity fade is greater when compared to 4.5 V as UCV. This increased rate of capacity fade, at higher UCV, is related to irreversible lattice contractions that leads to structural rearrangement at charged states during high-voltage cycling. Lastly, our results show a change in transition metal oxidation states and an onset of structural ordering occurs when the UCV is 4.7 V.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- OSTI Identifier:
- 1561675
- Alternate Identifier(s):
- OSTI ID: 1558680
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemElectroChem
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 22; Journal ID: ISSN 2196-0216
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Li-ion battery; Ni-rich cathodes; electrochemistry; magnetic susceptibility; in situ XRD
Citation Formats
David, Lamuel Abraham, Mohanty, Debasish, Geng, Linxiao, Ruther, Rose E., Sefat, Athena Safa, Cakmak, Ercan, Veith, Gabriel M., Meyer, III, Harry M., Wang, Hsin, and Wood, III, David L. High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation. United States: N. p., 2019.
Web. doi:10.1002/celc.201901338.
David, Lamuel Abraham, Mohanty, Debasish, Geng, Linxiao, Ruther, Rose E., Sefat, Athena Safa, Cakmak, Ercan, Veith, Gabriel M., Meyer, III, Harry M., Wang, Hsin, & Wood, III, David L. High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation. United States. https://doi.org/10.1002/celc.201901338
David, Lamuel Abraham, Mohanty, Debasish, Geng, Linxiao, Ruther, Rose E., Sefat, Athena Safa, Cakmak, Ercan, Veith, Gabriel M., Meyer, III, Harry M., Wang, Hsin, and Wood, III, David L. Fri .
"High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation". United States. https://doi.org/10.1002/celc.201901338. https://www.osti.gov/servlets/purl/1561675.
@article{osti_1561675,
title = {High-Voltage Performance of Ni-Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation},
author = {David, Lamuel Abraham and Mohanty, Debasish and Geng, Linxiao and Ruther, Rose E. and Sefat, Athena Safa and Cakmak, Ercan and Veith, Gabriel M. and Meyer, III, Harry M. and Wang, Hsin and Wood, III, David L.},
abstractNote = {High-voltage Ni-rich cathodes have been studied as a possible way to achieve high energy density in Li-ion batteries. However, capacity fade due to structural changes at high voltages has limited their applications. In this study, we identify 4.5 V (vs. graphite) as the optimum upper cutoff voltage (UCV) for a Ni-rich NCA cathode [LiNi0.8Co0.15Al0.05O2]. At this UCV, NCA delivers a 12 % increase in reversible capacity (when discharged to 2.5 V) and retains 92 % of its initial capacity after 100 cycles at 1C/-1C cycling when compared to 4.2 V as UCV. By increasing UCV to 4.7 V, the discharge capacity can be raised to >200 mAh/g. However, the rate of capacity fade is greater when compared to 4.5 V as UCV. This increased rate of capacity fade, at higher UCV, is related to irreversible lattice contractions that leads to structural rearrangement at charged states during high-voltage cycling. Lastly, our results show a change in transition metal oxidation states and an onset of structural ordering occurs when the UCV is 4.7 V.},
doi = {10.1002/celc.201901338},
journal = {ChemElectroChem},
number = 22,
volume = 6,
place = {United States},
year = {Fri Aug 16 00:00:00 EDT 2019},
month = {Fri Aug 16 00:00:00 EDT 2019}
}
Web of Science
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