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Synthesis, phases, structures, and electrical properties of melilite-type La1+xSr1−xGa3S6O1+0.5x materials

  • Lijia Zhou
  • Shipeng Geng
  • Xue Fang
  • Jungu XuEmail author
Original Paper


Deformation flexibility of two-dimensionally connected tetrahedral network and Ga3+ ion with variable coordination are reported to be the key factor for oxide ion migration in La1+xSr1−xGa3O7+0.5x materials, which are well-known oxide ion conductors with remarkable conductivity at the temperature range 600–900 °C. In this work, La1+xSr1−xGa3S6O1+0.5x materials which also adapt melilite structure were prepared at high temperature in a quartz tube after being vacuumed. The prepared samples were then studied by complementary techniques, including X-ray diffraction (XRD), alternative current (AC) impedance spectroscopy, and density functional theory (DFT). The XRD data together with Rietveld refinement results showed that La atoms failed to replace Sr atoms in La1+xSr1−xGa3S6O1+0.5x materials, leading to two phases in the products. This was consistent with the high defect formation energy (higher than 2.76 eV) of La atoms substituting for Sr atoms. In addition, alternative current impedance spectroscopy measurements demonstrated no ionic conduction responses in these melilite La1+xSr1−xGa3S6O1+0.5x materials, agreeing well with the fact that the La atoms were not able to substitute for Sr atoms and no interstitial oxide ions were introduced in any phases of the products.


Melilite Oxysulfates Oxide ion conductors Defect formation energy 


Funding information

This study was financially supported by National Natural Science Foundation of China (No. 21601040, No. 21622101) and Guangxi Natural Science Foundation (2017GXNSFAA198203).


  1. 1.
    Kuang X, Payne JL, Johnson MR, Radosavljevic Evans I (2012) Remarkably high oxide ion conductivity at low temperature in an ordered fluorite-type superstructure. Angew Chem Int Ed 51:690–694CrossRefGoogle Scholar
  2. 2.
    Malavasi L, Fisher CA, Islam MS (2010) Oxide-ion and proton conducting electrolyte materials for clean energy applications: structural and mechanistic features. Chem Soc Rev 39:4370–4387CrossRefPubMedGoogle Scholar
  3. 3.
    Steele B, Heinzel A (2001) Materials for fuel-cell technologies. Nature 414:345–352CrossRefGoogle Scholar
  4. 4.
    Boivin JC, Mairesse G (1998) Recent material development in fast oxide ion conductors. Chem Mater 10:2870–2888CrossRefGoogle Scholar
  5. 5.
    Arikawa H, Nishiguchi H, Ishihara T, Takita Y (2000) Oxide ion conductivity in Sr-doped La10Ge6O27 apatite oxide. Solid State Ionics 136:31–37CrossRefGoogle Scholar
  6. 6.
    Islam MS, Tolchard JR, Slater PR (2003) An apatite for fast oxide ion conduction. Chem Commun 2:1486–1487CrossRefGoogle Scholar
  7. 7.
    León-Reina L, Losilla ER, Martínez-Lara M, Bruque S, Aranda MAG (2004) Interstitial oxygen conduction in lanthanum oxy-apatite electrolytes. J Mater Chem 14:1142–1149CrossRefGoogle Scholar
  8. 8.
    León-Reina L, Losilla ER, Martínez-Lara M, Martín-Sedeño MC, Bruque S, Núñez P, Sheptyakov DV, Aranda MAG (2005) High oxide ion conductivity in Al-doped germanium oxyapatite. Chem Mater 17:596–600CrossRefGoogle Scholar
  9. 9.
    Esaka T, Mina-Ai T, Iwahara H (1992) Oxide ion conduction in the solid solution based on the scheelite-type oxide PbWO4. Solid State Ionics 57:319–325CrossRefGoogle Scholar
  10. 10.
    Lacerda M, Irvine JTS, Glasser FP, West AR (1998) High oxide ion conductivity in Ca12Al14O33. Nature 332:525–526CrossRefGoogle Scholar
  11. 11.
    Kuang X, Green MA, Niu H, Zajdel P, Dickinson C, Claridge JB, Jantsky L, Rosseinsky MJ (2008) Interstitial oxide ion conductivity in the layered tetrahedral network melilite structure. Nature material 7:498–504CrossRefGoogle Scholar
  12. 12.
    Yu RJ, Park JY, Yang HK, Moon BK, Choi BC, Jeong JH (2012) A new deep red-emitting Mn2+-activated SrLaGa3S6O phosphor. Key Eng Mater 531-532:145–148CrossRefGoogle Scholar
  13. 13.
    Zhang G, Cui Q, Liu G (2016) Efficient near-infrared quantum cutting and downshift in Ce3+-Pr3+ codoped SrLaGa3S6O suitable for solar spectral converter. Opt Mater 53:214–217CrossRefGoogle Scholar
  14. 14.
    Yu R, Deng B, Zhang G, An Y, Zhang J, Wang J (2011) Luminescence properties of Ce3+-activated SrLaGa3S6O and application in white LEDs. J Electrochem Soc 158:J255–J259CrossRefGoogle Scholar
  15. 15.
    Zhang X, Zhang J, Xu J, Su Q (2005) Luminescent properties of Eu2+-activated SrLaGa3S6O phosphor. J Alloys Compd 389:247–251CrossRefGoogle Scholar
  16. 16.
    Yu R et al (2008) A new blue-emitting phosphor of Ce3+-activated CaLaGa3S6O for white-light-emitting diodes. Chem Phys Lett 453:197–201CrossRefGoogle Scholar
  17. 17.
    Gongguo Z, Jing W, Yan C, Qiang S (2010) Two-color emitting of Ce3+ and Tb3+ co-doped CaLaGa3S6O for UV LEDs. Opt Lett 35:2382–2384CrossRefGoogle Scholar
  18. 18.
    Zhu J, Qin S, Xia Z, Liu Q (2015) Synthesis and color-tunable emission studies of Y2Si3O3N4:Ce3+,Tb3+ phosphors. Ceram Int 41:12633–12637CrossRefGoogle Scholar
  19. 19.
    Xu J, Wang J, Tang X, Kuang X, Rosseinsky MJ (2017) La1+xBa1-xGa3O7+0.5x oxide ion conductor: cationic size effect on the interstitial oxide ion conductivity in gallate melilites. Inorg Chem 56:6897–6905CrossRefPubMedGoogle Scholar
  20. 20.
    Bayliss RD et al (2014) Understanding the defect chemistry of alkali metal strontium silicate solid solutions: insights from experiment and theory. Journal of Materials Chemisry A 2:17919–17924CrossRefGoogle Scholar
  21. 21.
    Perdew JP, Burke K, Ernzerhof M (1996) Generalized gradient approximation made simple. Phys Rev Lett 77:3865–3868CrossRefPubMedGoogle Scholar
  22. 22.
    Ahrens LH (1952) The use of ionization potentials part 1. Ionic radii of the elements. Geochimica Et Cosmochimica Acta 2:155–169CrossRefGoogle Scholar
  23. 23.
    Johnson D (2002) ZView and ZPlot: a software program for IES analysis,Version 2.8. Scribner Associates, Inc., Southern PinesGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

  1. 1.MOE Key Laboratory of New Processing Technology for Nonferrous Metal and Materials, Guangxi Universities Key Laboratory of Non-Ferrous Metal Oxide Electronic Functional Materials and Devices, College of Materials Science and EngineeringGuilin University of TechnologyGuilinPeople’s Republic of China

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