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@ARTICLE{Schuett:1024909,
author = {Schuett, Judith and Kuhn, Antonia S. and
Neitzel-Grieshammer, Steffen},
title = {{P}redicting the {N}a + ion transport properties of
{N}a{SICON} materials using density functional theory and
{K}inetic {M}onte {C}arlo},
journal = {Journal of materials chemistry / A},
volume = {11},
number = {16},
issn = {2050-7488},
address = {London [u.a.]},
publisher = {RSC},
reportid = {FZJ-2024-02559},
pages = {9160 - 9177},
year = {2023},
abstract = {The efficiency of all-solid-state Na+ ion batteries
crucially depends on the applied electrolyte, among which
sodium super ionic conductors (NaSICONs) show high ionic
conductivities. However, the experimental data on ionic
conductivities available in the literature vary by several
orders of magnitude depending on composition and sample
preparation. Hence, a comprehensive understanding of Na+
transport properties is still lacking. In this study, we
investigate the multi-cationic NaSICONs Na1+xM2SixP3−xO12
(with M = Zr4+, Hf4+, Sn4+, and 0 ≤ x ≤ 3) by combining
state-of-the-art computational tools, namely density
functional theory calculations to analyse the structure at
the atomic level and Kinetic Monte Carlo simulations to
study the ion transport on the macroscopic level. The
results show that there is no simple correlation between
structural properties and the Na+ ion transport as often
described in the literature. Rather the interplay of the
ratio of unoccupied to occupied charge carrier sites,
interactions between Na+ ions and adjacent cations, and Na+
migration barriers, which are influenced by both the
M-cation and the degree of substitution, must be considered.
Our study provides a detailed picture of the complex ion
transport in NaSICONs of variable composition.},
cin = {IEK-12},
ddc = {530},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {1221 - Fundamentals and Materials (POF4-122)},
pid = {G:(DE-HGF)POF4-1221},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000969590000001},
doi = {10.1039/D3TA00440F},
url = {https://juser.fz-juelich.de/record/1024909},
}