TY  - JOUR
AU  - Böger, Thorben
AU  - Bernges, Tim
AU  - Agne, Matthias T.
AU  - Canepa, Pieremanuele
AU  - Tietz, Frank
AU  - Zeier, Wolfgang G.
TI  - On the Thermal Conductivity and Local Lattice Dynamical Properties of NASICON Solid Electrolytes
JO  - Journal of the American Chemical Society
VL  - 146
IS  - 47
SN  - 0002-7863
CY  - Washington, DC
PB  - ACS Publications
M1  - FZJ-2024-06270
SP  - 32678 - 32688
PY  - 2024
N1  - Funded by the European Union (ERC, DIONISOS, 101123802), Deutsche Forschungsgemeinschaft (DFG) under project number 459785385
AB  - 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.
LB  - PUB:(DE-HGF)16
C6  - 39537339
UR  - <Go to ISI:>//WOS:001354941200001
DO  - DOI:10.1021/jacs.4c12034
UR  - https://juser.fz-juelich.de/record/1032477
ER  -