NaSICON-type solid-state Li+ ion conductors with partial polyanionic substitution of phosphate with silicate

The increasing demand for safe energy storage has led to intensive investigations of solid-state Li+-ion conductors in the Li2O-M2O3–ZrO2–SiO2–P2O5 system. As a continuation of the cation substitution in this system, which we reported on very recently, a study of the impact of polyanionic substituti...

Full description

Bibliographic Details
Main Authors: Asmaa Loutati, Olivier Guillon, Frank Tietz, Dina Fattakhova-Rohlfing
Format: Article
Language:English
Published: Elsevier 2022-12-01
Series:Open Ceramics
Subjects:
Online Access:http://www.sciencedirect.com/science/article/pii/S2666539522000967
_version_ 1797987487465865216
author Asmaa Loutati
Olivier Guillon
Frank Tietz
Dina Fattakhova-Rohlfing
author_facet Asmaa Loutati
Olivier Guillon
Frank Tietz
Dina Fattakhova-Rohlfing
author_sort Asmaa Loutati
collection DOAJ
description The increasing demand for safe energy storage has led to intensive investigations of solid-state Li+-ion conductors in the Li2O-M2O3–ZrO2–SiO2–P2O5 system. As a continuation of the cation substitution in this system, which we reported on very recently, a study of the impact of polyanionic substitutions on ionic conductivity was carried out here in two series, Li3+xSc2SixP3-xO12 (0 ≤ x ≤ 0.6) and Li1.2+xSc0.2Zr1.8SixP3-xO12 (0.3 ≤ x ≤ 2.8), with the aim of increasing ionic conductivity, determing the phase stability, and optimizing the processing conditions – especially decreasing the sintering temperatures – depending on the level of substitution.The polyanionic substitution, i.e. the substitution of (PO4)3- with (SiO4)4-, in the Li2O–Sc2O3–ZrO2–SiO2–P2O5 system revealed that a) the sintering temperature can effectively be reduced, b) the presence of zirconium can limit the evaporation of lithium species even at high sintering temperatures, c) the purity of the NaSICON materials has a strong influence on the grain boundary resistance, and therefore on the ionic conductivity, and d) the silicate substitution in Li3+xSc2SixP3-xO12 (0 ≤ x ≤ 0.6) stabilized the monoclinic polymorph (space group P21/n) with an enhanced total ionic conductivity at 25 °C from 6.5 × 10−7 S cm−1 to 1.2 × 10−5 S cm−1 for x = 0 to x = 0.15, respectively, exhibiting the highest ionic conductivity at 25 °C among the compositions investigated.
first_indexed 2024-04-11T07:49:14Z
format Article
id doaj.art-372c76cd835f4e1d9970902e0d3f0bb6
institution Directory Open Access Journal
issn 2666-5395
language English
last_indexed 2024-04-11T07:49:14Z
publishDate 2022-12-01
publisher Elsevier
record_format Article
series Open Ceramics
spelling doaj.art-372c76cd835f4e1d9970902e0d3f0bb62022-12-22T04:36:09ZengElsevierOpen Ceramics2666-53952022-12-0112100313NaSICON-type solid-state Li+ ion conductors with partial polyanionic substitution of phosphate with silicateAsmaa Loutati0Olivier Guillon1Frank Tietz2Dina Fattakhova-Rohlfing3Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research, Materials Synthesis and Processing (IEK-1), D-52425, Jülich, Germany; Forschungszentrum Jülich GmbH, Helmholtz-Institute Münster (IEK-12), D-52425, Jülich, Germany; University of Duisburg-Essen, Faculty of Engineering, Lotharstr. 1, 47057, Duisburg, Germany; Corresponding author. Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research, Materials Synthesis and Processing (IEK-1), D-52425, Jülich, Germany.Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research, Materials Synthesis and Processing (IEK-1), D-52425, Jülich, Germany; Forschungszentrum Jülich GmbH, Helmholtz-Institute Münster (IEK-12), D-52425, Jülich, Germany; Jülich Aachen Research Alliance, JARA-ENERGY, GermanyForschungszentrum Jülich GmbH, Institute of Energy and Climate Research, Materials Synthesis and Processing (IEK-1), D-52425, Jülich, Germany; Forschungszentrum Jülich GmbH, Helmholtz-Institute Münster (IEK-12), D-52425, Jülich, GermanyForschungszentrum Jülich GmbH, Institute of Energy and Climate Research, Materials Synthesis and Processing (IEK-1), D-52425, Jülich, Germany; Forschungszentrum Jülich GmbH, Helmholtz-Institute Münster (IEK-12), D-52425, Jülich, Germany; University of Duisburg-Essen, Faculty of Engineering, Lotharstr. 1, 47057, Duisburg, GermanyThe increasing demand for safe energy storage has led to intensive investigations of solid-state Li+-ion conductors in the Li2O-M2O3–ZrO2–SiO2–P2O5 system. As a continuation of the cation substitution in this system, which we reported on very recently, a study of the impact of polyanionic substitutions on ionic conductivity was carried out here in two series, Li3+xSc2SixP3-xO12 (0 ≤ x ≤ 0.6) and Li1.2+xSc0.2Zr1.8SixP3-xO12 (0.3 ≤ x ≤ 2.8), with the aim of increasing ionic conductivity, determing the phase stability, and optimizing the processing conditions – especially decreasing the sintering temperatures – depending on the level of substitution.The polyanionic substitution, i.e. the substitution of (PO4)3- with (SiO4)4-, in the Li2O–Sc2O3–ZrO2–SiO2–P2O5 system revealed that a) the sintering temperature can effectively be reduced, b) the presence of zirconium can limit the evaporation of lithium species even at high sintering temperatures, c) the purity of the NaSICON materials has a strong influence on the grain boundary resistance, and therefore on the ionic conductivity, and d) the silicate substitution in Li3+xSc2SixP3-xO12 (0 ≤ x ≤ 0.6) stabilized the monoclinic polymorph (space group P21/n) with an enhanced total ionic conductivity at 25 °C from 6.5 × 10−7 S cm−1 to 1.2 × 10−5 S cm−1 for x = 0 to x = 0.15, respectively, exhibiting the highest ionic conductivity at 25 °C among the compositions investigated.http://www.sciencedirect.com/science/article/pii/S2666539522000967CeramicsLi solid electrolyteNaSICONAnion substitutionImpedance spectroscopyIonic conductivity
spellingShingle Asmaa Loutati
Olivier Guillon
Frank Tietz
Dina Fattakhova-Rohlfing
NaSICON-type solid-state Li+ ion conductors with partial polyanionic substitution of phosphate with silicate
Open Ceramics
Ceramics
Li solid electrolyte
NaSICON
Anion substitution
Impedance spectroscopy
Ionic conductivity
title NaSICON-type solid-state Li+ ion conductors with partial polyanionic substitution of phosphate with silicate
title_full NaSICON-type solid-state Li+ ion conductors with partial polyanionic substitution of phosphate with silicate
title_fullStr NaSICON-type solid-state Li+ ion conductors with partial polyanionic substitution of phosphate with silicate
title_full_unstemmed NaSICON-type solid-state Li+ ion conductors with partial polyanionic substitution of phosphate with silicate
title_short NaSICON-type solid-state Li+ ion conductors with partial polyanionic substitution of phosphate with silicate
title_sort nasicon type solid state li ion conductors with partial polyanionic substitution of phosphate with silicate
topic Ceramics
Li solid electrolyte
NaSICON
Anion substitution
Impedance spectroscopy
Ionic conductivity
url http://www.sciencedirect.com/science/article/pii/S2666539522000967
work_keys_str_mv AT asmaaloutati nasicontypesolidstateliionconductorswithpartialpolyanionicsubstitutionofphosphatewithsilicate
AT olivierguillon nasicontypesolidstateliionconductorswithpartialpolyanionicsubstitutionofphosphatewithsilicate
AT franktietz nasicontypesolidstateliionconductorswithpartialpolyanionicsubstitutionofphosphatewithsilicate
AT dinafattakhovarohlfing nasicontypesolidstateliionconductorswithpartialpolyanionicsubstitutionofphosphatewithsilicate