Chemical trends in the lattice thermal conductivity of Li(Ni, Mn, Co)O-2 (NMC) battery cathodes
File(s)thermal_NMC.pdf (2.4 MB)
Accepted version
Author(s)
Type
Journal Article
Abstract
While the transport of ions and electrons in conventional Li-ion battery cathode materials is well understood, our knowledge of the phonon (heat) transport is still in its infancy. We present a first-principles theoretical investigation of the chemical trends in the phonon frequency dispersion, mode lifetimes, and thermal conductivity in the series of layered lithium transition-metal oxides Li(NixMnyCoz)O2 (x + y + z = 1). The oxidation and spin states of the transition metal cations are found to strongly influence the structural dynamics. Calculations of the thermal conductivity show that LiCoO2 has highest average conductivity of 45.9 W·m–1·K–1 at T = 300 K and the largest anisotropy, followed by LiMnO2 with 8.9 W·m–1·K–1 and LiNiO2 with 6.0 W·m–1·K–1. The much lower thermal conductivity of LiMnO2 and LiNiO2 is found to be due to 1–2 orders of magnitude shorter phonon lifetimes. We further model the properties of binary and ternary transition metal combinations to examine the possible effects of mixing on the thermal transport. These results serve as a guide to ongoing work on the design of multicomponent battery electrodes with more effective thermal management.
Date Issued
2020-09-08
Date Acceptance
2020-07-28
Citation
Chemistry of Materials, 2020, 32 (17), pp.7542-7550
ISSN
0897-4756
Publisher
American Chemical Society
Start Page
7542
End Page
7550
Journal / Book Title
Chemistry of Materials
Volume
32
Issue
17
Copyright Statement
© 2020 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.chemmater.0c02908
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000569075300044&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Materials Science, Multidisciplinary
Chemistry
Materials Science
ELECTROCHEMICAL PROPERTIES
ION BATTERY
LITHIUM
THERMODYNAMICS
LICOO2
CO
Publication Status
Published
Date Publish Online
2020-07-28