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@ARTICLE{Bger:1032477,
author = {Böger, Thorben and Bernges, Tim and Agne, Matthias T. and
Canepa, Pieremanuele and Tietz, Frank and Zeier, Wolfgang
G.},
title = {{O}n the {T}hermal {C}onductivity and {L}ocal {L}attice
{D}ynamical {P}roperties of {NASICON} {S}olid
{E}lectrolytes},
journal = {Journal of the American Chemical Society},
volume = {146},
number = {47},
issn = {0002-7863},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {FZJ-2024-06270},
pages = {32678 - 32688},
year = {2024},
note = {Funded by the European Union (ERC, DIONISOS, 101123802),
Deutsche Forschungsgemeinschaft (DFG) under project number
459785385},
abstract = {The recent development of solid-state batteries brings them
closer to commercialization and raises the need for heat
management. The NASICON material class
($Na_{1+x}Zr_2P_xSi_{3–x}O_{12}$ with 0 ≤ x ≤ 3) is
one of the most promising families of solid electrolytes for
sodium solid-state batteries. While extensive research has
been conducted to improve the ionic conductivity of this
material class, knowledge of thermal conductivity is scarce.
At the same time, the material’s ability to dissipate heat
is expected to play a pivotal role in determining efficiency
and safety, both on a battery pack and local component
level. Dissipation of heat, which was, for instance,
generated during battery operation, is important to keep the
battery at its optimal operating temperature and avoid
accelerated degradation of battery materials at interfaces.
In this study, the thermal conductivity of $NaZr_2P_3O_{12}$
and $Na_4Zr_2Si_3O_{12}$ is investigated in a wide
temperature range from 2 to 773 K accompanied by in-depth
lattice dynamical characterizations to understand underlying
mechanisms and the striking difference in their
low-temperature thermal conductivity. Consistently low
thermal conductivities are observed, which can be explained
by the strong suppression of propagating phonon transport
through the structural complexity and the intrinsic
anharmonicity of NASICONs. The associated low-frequency
sodium ion vibrations lead to the emergence of local
random-walk heat transport contributions via so-called
diffusons. In addition, the importance of lattice dynamics
in the discussion of ionic transport as well as the
relevance of bonding characteristics typical for mobile ions
on thermal transport, is highlighted.},
cin = {IMD-4},
ddc = {540},
cid = {I:(DE-Juel1)IMD-4-20141217},
pnm = {1221 - Fundamentals and Materials (POF4-122)},
pid = {G:(DE-HGF)POF4-1221},
typ = {PUB:(DE-HGF)16},
pubmed = {39537339},
UT = {WOS:001354941200001},
doi = {10.1021/jacs.4c12034},
url = {https://juser.fz-juelich.de/record/1032477},
}