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@ARTICLE{Loutati:912434,
author = {Loutati, Asmaa and Odenwald, Philipp and Aktekin, Burak and
Sann, Joachim and Guillon, Olivier and Tietz, Frank and
Fattakhova-Rohlfing, Dina},
title = {{S}urvey of {Z}irconium‐{C}ontaining {N}a{SICON}‐type
{S}olid‐{S}tate {L}i+ {I}on {C}onductors with the {A}im of
{I}ncreasing {R}eduction {S}tability by {P}artial {C}ation
{S}ubstitution},
journal = {Batteries $\&$ supercaps},
volume = {5},
number = {11},
issn = {2566-6223},
address = {Weinheim},
publisher = {Wiley-VCH},
reportid = {FZJ-2022-05613},
pages = {e202200327},
year = {2022},
note = {Grand names: BMBF-03XP0173A Kompetenzcluster
Festbatt-OxideBMBF-13XP0434A Kompetenzcluster
Festbatt2-Oxide},
abstract = {Various compositions of the series Li1+xM3+xZr2−x(PO4)3
where M3+=Al3+, Sc3+, Y3+ were prepared by solution-assisted
solid-state reaction, since they could have a higher
reduction stability as solid electrolytes in lithium
batteries than in germanium- or titanium-containing
materials. The influence of substitution on crystallographic
parameters, density, and ionic conductivity were
investigated. The cation substitution of M3+ (M=Al, Sc, Y)
for Zr4+ in LiZr2(PO4)3 stabilizes the rhombohedral NaSICON
structure (space group
urn:x-wiley:25666223:media:batt202200327:batt202200327-math-0001
) at room temperature and increases the ionic conductivity
significantly. Here, at 25 °C and with a consistent
relative density of $94 \%–96 \%,$ an ionic
conductivity of 2.7×10−5 S cm−1,
6.7×10−5 S cm−1, and 3.6×10−6 S cm−1 was
achieved with the compositions Li1.2Sc0.2Zr1.8(PO4)3,
Li1.2Y0.2Zr1.8(PO4)3, and Li1.2Al0.2Zr1.8(PO4)3,
respectively. In comparison with Li1+xScxZr2−x(PO4)3, the
Y3+ substitution in LiZr2(PO4)3 enhanced the ionic
conductivity slightly and denoted the maximum Li+ ionic
conductivity obtained at room temperature. However,
substitution with Al3+ decreased the ionic conductivity. For
the first time, this work provides a complete overview of
three series of solid Li-ion conductors in the
Li2O-M2O3-ZrO2-P2O5 system where M=Al, Sc, Y. Noticeable
differences in the chemistry of resulting compounds were
observed, which likely depend on the ionic radius of the
cations being substituted. The series with Sc showed
complete miscibility from x=0 to x=2 with a continuous
change of the NaSICON polymorphs. The series with Y showed a
solubility limit at about x=0.3 and higher substitution
levels led to the increasing formation of YPO4. The series
with Al exhibited continuously decreasing ionic conductivity
until x=1, whereupon the investigation was terminated due to
its very low conductivity of about 10−10 S cm−1.},
cin = {IEK-1 / IEK-12},
ddc = {620},
cid = {I:(DE-Juel1)IEK-1-20101013 / 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:000853914500001},
doi = {10.1002/batt.202200327},
url = {https://juser.fz-juelich.de/record/912434},
}