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000912434 0247_ $$2doi$$a10.1002/batt.202200327
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000912434 1001_ $$0P:(DE-Juel1)165315$$aLoutati, Asmaa$$b0$$eCorresponding author
000912434 245__ $$aSurvey of Zirconium‐Containing NaSICON‐type Solid‐State Li+ Ion Conductors with the Aim of Increasing Reduction Stability by Partial Cation Substitution
000912434 260__ $$aWeinheim$$bWiley-VCH$$c2022
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000912434 500__ $$aGrand names: BMBF-03XP0173A Kompetenzcluster Festbatt-OxideBMBF-13XP0434A Kompetenzcluster Festbatt2-Oxide
000912434 520__ $$aVarious 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.
000912434 536__ $$0G:(DE-HGF)POF4-1221$$a1221 - Fundamentals and Materials (POF4-122)$$cPOF4-122$$fPOF IV$$x0
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000912434 7001_ $$0P:(DE-Juel1)177015$$aOdenwald, Philipp$$b1
000912434 7001_ $$00000-0002-8659-7519$$aAktekin, Burak$$b2
000912434 7001_ $$00000-0003-4663-2671$$aSann, Joachim$$b3
000912434 7001_ $$0P:(DE-Juel1)161591$$aGuillon, Olivier$$b4
000912434 7001_ $$0P:(DE-Juel1)129667$$aTietz, Frank$$b5$$eCorresponding author
000912434 7001_ $$0P:(DE-Juel1)171780$$aFattakhova-Rohlfing, Dina$$b6
000912434 773__ $$0PERI:(DE-600)2897248-X$$a10.1002/batt.202200327$$gVol. 5, no. 11$$n11$$pe202200327$$tBatteries & supercaps$$v5$$x2566-6223$$y2022
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