Quantum prediction of ultra-low thermal conductivity in lithium intercalation materials
Abstract
Lithium-intercalated layered transition-metal oxides, LixTMO2, brought about a paradigm change in rechargeable batteries in recent decades and show promise for use in memristors, a type of device for future neural computing and on-chip storage. Thermal transport properties, although being a crucial element in limiting the charging/discharging rate, package density, energy efficiency, and safety of batteries as well as the controllability and energy consumption of memristors, are poorly managed or even understood yet. Here, for the first time, we employ quantum calculations including high-order lattice anharmonicity and find that the thermal conductivity κ of LixTMO2 materials is significantly lower than hitherto believed. More specifically, the theoretical upper limit of of LiCoO2 is 6 W/m-K, 2–6 times lower than the prior theoretical predictions. Delithiation further reduces by 40–70% for LiCoO2 and LiNbO2. Grain boundaries, strain, and porosity are yet additional causes of thermal-conductivity reduction, while Li-ion diffusion and electrical transport are found to have only a minor effect on phonon thermal transport. The results elucidate several long-standing issues regarding the thermal transport in lithium-intercalated materials and provide guidance toward designing high-energy-density batteries and controllable memristors.
- Authors:
-
[1];
[2];
[1]
- Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Vanderbilt Univ., Nashville, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1632076
- Alternate Identifier(s):
- OSTI ID: 1694288
- Grant/Contract Number:
- AC05-00OR22725; FG0209ER46554; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Energy
- Additional Journal Information:
- Journal Volume: 75; Journal Issue: C; Journal ID: ISSN 2211-2855
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE
Citation Formats
Feng, Tianli, O'Hara, Andrew, and Pantelides, Sokrates T. Quantum prediction of ultra-low thermal conductivity in lithium intercalation materials. United States: N. p., 2020.
Web. doi:10.1016/j.nanoen.2020.104916.
Feng, Tianli, O'Hara, Andrew, & Pantelides, Sokrates T. Quantum prediction of ultra-low thermal conductivity in lithium intercalation materials. United States. https://doi.org/10.1016/j.nanoen.2020.104916
Feng, Tianli, O'Hara, Andrew, and Pantelides, Sokrates T. Sat .
"Quantum prediction of ultra-low thermal conductivity in lithium intercalation materials". United States. https://doi.org/10.1016/j.nanoen.2020.104916. https://www.osti.gov/servlets/purl/1632076.
@article{osti_1632076,
title = {Quantum prediction of ultra-low thermal conductivity in lithium intercalation materials},
author = {Feng, Tianli and O'Hara, Andrew and Pantelides, Sokrates T.},
abstractNote = {Lithium-intercalated layered transition-metal oxides, LixTMO2, brought about a paradigm change in rechargeable batteries in recent decades and show promise for use in memristors, a type of device for future neural computing and on-chip storage. Thermal transport properties, although being a crucial element in limiting the charging/discharging rate, package density, energy efficiency, and safety of batteries as well as the controllability and energy consumption of memristors, are poorly managed or even understood yet. Here, for the first time, we employ quantum calculations including high-order lattice anharmonicity and find that the thermal conductivity κ of LixTMO2 materials is significantly lower than hitherto believed. More specifically, the theoretical upper limit of κ of LiCoO2 is 6 W/m-K, 2–6 times lower than the prior theoretical predictions. Delithiation further reduces κ by 40–70% for LiCoO2 and LiNbO2. Grain boundaries, strain, and porosity are yet additional causes of thermal-conductivity reduction, while Li-ion diffusion and electrical transport are found to have only a minor effect on phonon thermal transport. The results elucidate several long-standing issues regarding the thermal transport in lithium-intercalated materials and provide guidance toward designing high-energy-density batteries and controllable memristors.},
doi = {10.1016/j.nanoen.2020.104916},
journal = {Nano Energy},
number = C,
volume = 75,
place = {United States},
year = {Sat May 23 00:00:00 EDT 2020},
month = {Sat May 23 00:00:00 EDT 2020}
}
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