Highly Anisotropic Thermal Transport in LiCoO2

Hui Yang; Jia-Yue  Yang; Christopher Savory; Jonathan Skelton; Benjamin Morgan; David O Scanlon; Aron Walsh

doi:10.26434/chemrxiv.8874404.v2

Highly Anisotropic Thermal Transport in LiCoO₂

Hui Yang, Jia-Yue Yang, Christopher Savory, Jonathan Skelton, Benjamin Morgan, David O Scanlon, Aron Walsh

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

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Abstract

LiCoO ₂ is the prototypical cathode in lithium-ion batteries. Its crystal structure consists of Li ⁺ and CoO2 _- layers that alternate along the hexagonal «0001»axis. It is well established that the ionic and electronic conduction are anisotropic, but little is known regarding the heat transport. We analyze the phonon dispersion and lifetimes using anharmonic lattice dynamics based on quantum-chemical force constants. Around room temperature, the thermal conductivity in the hexagonal ab plane of the layered cathode is ∼6 times higher than that along the c axis. An upper limit to the average thermal conductivity at T = 300 K of 38.5 W m ^-1 K ^-1 is set by short phonon lifetimes associated with anharmonic interactions within the octahedral face-sharing CoO2 _- network. Observations of conductivity <10 W m ^-1 K ^-1 can be understood by additional scattering channels including grain boundaries in polycrystalline samples. The impact on thermal processes in lithium-ion batteries is discussed.

Original language	English
Pages (from-to)	5552-5556
Number of pages	5
Journal	Journal of Physical Chemistry Letters
Volume	10
Issue number	18
Early online date	1 Sept 2019
DOIs	https://doi.org/10.26434/chemrxiv.8874404.v2 https://doi.org/10.1021/acs.jpclett.9b02073
Publication status	Published - 19 Sept 2019

Bibliographical note

Funding Information:
This work was carried out with funding from the Faraday Institution ( faraday.ac.uk ; EP/S003053/1) grant number FIRG003 and used the MICHAEL computing cluster. We are also grateful for computer resources from RWTH Aachen. J.Y. is supported by Shandong University (Qilu Young Scholar 89963031). A.W. and B.J.M. are supported by Royal Society University Research Fellowships (Nos. UF100278 and UF130329). J.M.S. is supported by a Presidential Fellowship from the University of Manchester. Via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202), this work used the ARCHER UK National Supercomputing Service ( http://www.archer.ac.uk ).

ASJC Scopus subject areas

General Materials Science
Physical and Theoretical Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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thermal_LiCoO2Submitted manuscript, 1.14 MBLicence: CC BY-NC-ND
LiCoO2_Thermal_V2Submitted manuscript, 1.37 MBLicence: CC BY-NC-ND
acs.jpclett.9b02073
This document is the Accepted Manuscript version of a Published Work that appeared in final form in J. Phys. Chem. Lett., copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpclett.9b02073
Accepted author manuscript, 1.04 MB

Cite this

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abstract = "LiCoO 2 is the prototypical cathode in lithium-ion batteries. Its crystal structure consists of Li + and CoO2 - layers that alternate along the hexagonal «0001»axis. It is well established that the ionic and electronic conduction are anisotropic, but little is known regarding the heat transport. We analyze the phonon dispersion and lifetimes using anharmonic lattice dynamics based on quantum-chemical force constants. Around room temperature, the thermal conductivity in the hexagonal ab plane of the layered cathode is ∼6 times higher than that along the c axis. An upper limit to the average thermal conductivity at T = 300 K of 38.5 W m -1 K -1 is set by short phonon lifetimes associated with anharmonic interactions within the octahedral face-sharing CoO2 - network. Observations of conductivity <10 W m -1 K -1 can be understood by additional scattering channels including grain boundaries in polycrystalline samples. The impact on thermal processes in lithium-ion batteries is discussed. ",

author = "Hui Yang and Jia-Yue Yang and Christopher Savory and Jonathan Skelton and Benjamin Morgan and Scanlon, {David O} and Aron Walsh",

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N2 - LiCoO 2 is the prototypical cathode in lithium-ion batteries. Its crystal structure consists of Li + and CoO2 - layers that alternate along the hexagonal «0001»axis. It is well established that the ionic and electronic conduction are anisotropic, but little is known regarding the heat transport. We analyze the phonon dispersion and lifetimes using anharmonic lattice dynamics based on quantum-chemical force constants. Around room temperature, the thermal conductivity in the hexagonal ab plane of the layered cathode is ∼6 times higher than that along the c axis. An upper limit to the average thermal conductivity at T = 300 K of 38.5 W m -1 K -1 is set by short phonon lifetimes associated with anharmonic interactions within the octahedral face-sharing CoO2 - network. Observations of conductivity <10 W m -1 K -1 can be understood by additional scattering channels including grain boundaries in polycrystalline samples. The impact on thermal processes in lithium-ion batteries is discussed.

AB - LiCoO 2 is the prototypical cathode in lithium-ion batteries. Its crystal structure consists of Li + and CoO2 - layers that alternate along the hexagonal «0001»axis. It is well established that the ionic and electronic conduction are anisotropic, but little is known regarding the heat transport. We analyze the phonon dispersion and lifetimes using anharmonic lattice dynamics based on quantum-chemical force constants. Around room temperature, the thermal conductivity in the hexagonal ab plane of the layered cathode is ∼6 times higher than that along the c axis. An upper limit to the average thermal conductivity at T = 300 K of 38.5 W m -1 K -1 is set by short phonon lifetimes associated with anharmonic interactions within the octahedral face-sharing CoO2 - network. Observations of conductivity <10 W m -1 K -1 can be understood by additional scattering channels including grain boundaries in polycrystalline samples. The impact on thermal processes in lithium-ion batteries is discussed.

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Highly Anisotropic Thermal Transport in LiCoO₂

Abstract

Bibliographical note

ASJC Scopus subject areas

UN SDGs

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Faraday Institute Call - Multi-Scale Modelling

High Performance Computing (HPC) Facility

Cite this

Highly Anisotropic Thermal Transport in LiCoO2

Abstract

Bibliographical note

ASJC Scopus subject areas

UN SDGs

Access to Document

Other files and links

Fingerprint

Projects

Faraday Institute Call - Multi-Scale Modelling

Equipment

High Performance Computing (HPC) Facility

Cite this

Highly Anisotropic Thermal Transport in LiCoO₂