Journal of the Australian Ceramic Society

, Volume 54, Issue 2, pp 307–316 | Cite as

Structural, electrical conductivity and dielectric relaxation behavior of LiHf2(PO4)3 ceramic powders

  • Tasiu Zangina
  • Jumiah Hassan
  • Raba’ah Syahidah Azis
  • Khamirul Amin Matori
  • Alex See
  • Ibrahim Mustapha Alibe
  • Sadiq Umar
Research
  • 38 Downloads

Abstract

Lithium hafnium phosphate LiHf2(PO4)3 (LHP) was synthesized via solid-state synthesis technique. The sintering behavior, structure, and phase composition of the as-prepared sample was analyzed using X-ray diffraction (XRD) characterization technique. The XRD-Rietveld refinement analysis showed that after sintering at low temperatures 500 to 1000 °C, it exhibited various secondary phases. However, a single phase was observed as the sintering temperature increases from 1100 to 1200 °C. LHP sintered at 1100 °C produced real features of sodium superionic conductor type (NASICON-type) with hexagonal crystal axis indicating R-3c space group. The electrical properties were studied using impedance spectroscopy technique. Frequency and temperature dependence behavior of conductivity (ac and dc) and dielectric permittivity were studied. The results obtained describes the conduction mechanism in the system. Electric modulus formalism was performed to investigate the relaxation behavior which showed that as measuring temperature increases, the relaxation frequency increases whereas relaxation time decreases. This behavior explains the hopping mechanism of the charge carriers in the system. Likewise, the correlated barrier hopping model elucidates the dominant hopping mechanism.

Keywords

LiHf2(PO4)3 ceramics NASICON structure Conductivity Dielectric relaxation properties 

Notes

Acknowledgements

The authors gratefully acknowledge the Department of Physics, Faculty of Science, Universiti Putra Malaysia (UPM) for the facilities provided.

Funding information

This research work was supported financially by the Fundamental Research Grant Scheme (FRGS) Project No. 01-02-14-1599FR.

References

  1. 1.
    Arbi, K., Bucheli, W., Jiménez, R., Sanz, J.: High lithium ion conducting solid electrolytes based on NASICON Li 1+ xAlxM2− x(PO4)3 materials (M= Ti, Ge and 0≤ x≤ 0.5). J Eur Ceram Soc. 35, 1477–1484 (2015)CrossRefGoogle Scholar
  2. 2.
    Hiromichi Aono, E.S.: Electrical properties and crystal structure of solid electrolyte based on lithium hafnium phosphate LiHf2(PO4)3. Solid State Ionics. 62, 309–316 (1993)CrossRefGoogle Scholar
  3. 3.
    Aono, H., Sugimoto, E., Sadaoka, Y., Imanaka, N., Adachi, G.: Electrical property and sinterability of LiTi2(PO4)3 mixed with lithium salt (Li3PO4 or Li3BO3). Solid State Ionics. 47, 257–264 (1991)CrossRefGoogle Scholar
  4. 4.
    Maldonado-Manso, P., Aranda, M.A.G., Bruque, S., Sanz, J., Losilla, E.R.: Nominal vs. actual stoichiometries in Al-doped NASICONs: a study of the Na1.4Al0.4M1.6(PO4)3 (M = Ge, Sn, Ti, Hf, Zr) family. Solid State Ionics. 176, 1613–1625 (2005)CrossRefGoogle Scholar
  5. 5.
    Savitha, T., Selvasekarapandian, S., Ramya, C.S., Bhuvaneswari, M.S., Angelo, P.C.: Electrical conduction and relaxation mechanism in Li2AlZr[PO4]3. J Mater Sci. 42, 5470–5475 (2007)CrossRefGoogle Scholar
  6. 6.
    Thangadurai, V., Shukla, A.K., Gopalakrishnan, J.: New lithium-ion conductors based on the NASICON structure. J Mater Chem. 9, 739–741 (1999)CrossRefGoogle Scholar
  7. 7.
    Robertson, A., West, A., Ritchie, A.: Review of crystalline lithium-ion conductors suitable for high-temperature battery applications. Solid State Ionics. 104, 1–11 (1997)CrossRefGoogle Scholar
  8. 8.
    Chang, C., Hong, S., Park, H.: Spark plasma sintering of Al-substituted LiHf2 (PO4)3 solid electrolytes. Solid State Ionics. 176, 2583–2587 (2005)CrossRefGoogle Scholar
  9. 9.
    Enrique, L.M., Losillaa, R., Bruquea, S.’n., Arandaa, M.A.G., Real, L.M., Morin, E., Quarton, A.: NASICON to scandium wolframate transition in Li M Hf (PO) (M5Cr, Fe): structure and ionic conductivity. Solid State Ionics. 112(1), 53–62 (1998)Google Scholar
  10. 10.
    Ramaraghavulu, R., Buddhudu, S.: Analysis of structural, thermal and dielectric properties of LiTi2(PO4)3 ceramic powders. Ceram Int. 37, 3651–3656 (2011)CrossRefGoogle Scholar
  11. 11.
    Vijayan, L., Govindaraj, G.: Impedance spectroscopic studies of planetary ball-milled lithium titanium phosphate material. Phys B Condens Matter. 404, 3539–3543 (2009)CrossRefGoogle Scholar
  12. 12.
    Migahed, M.D., Ishra, M., Fahmy, T., Barakat, A.: Electric modulus and AC conductivity studies in conducting PPy composite films at low temperature. J Phys Chem Solids. 6, 1121–1125 (2004)CrossRefGoogle Scholar
  13. 13.
    París, M.A., Martínez-Juárez, A., Iglesias, J.E., Rojo, J.M., Sanz, J.: Phase transition and ionic mobility in LiHf2(PO4)3 with NASICON structure. Chem Mater. 9, 1430–1436 (1997)CrossRefGoogle Scholar
  14. 14.
    Gwier, E.L., Martinez-jutiez, A., Iglesias, J.E., Rojo, M.: Ionic conductivity of NASICON-type LiHf2(PO4)3: a reexamination. Solid State Ionics. 91, 295–301 (1996)CrossRefGoogle Scholar
  15. 15.
    Gaber, A., Abdel-Rahim, M.A., Abdel-Latief, A.Y., Abdel-Salam, M.N.: Influence of calcination temperature on the structure and porosity of nanocrystalline SnO2 synthesized by a conventional precipitation method. Int J Electrochem Sci. 9(1), 81–95 (2014)Google Scholar
  16. 16.
    Sun, F., Wang, R., Jiang, H., Zhou, W.: Synthesis of sodium titanium phosphate at ultra-low temperature. Res Chem Intermed. 39, 1857–1864 (2013)CrossRefGoogle Scholar
  17. 17.
    Anuar, N.K., Adnan, S.B.R.S., Mohamed, N.S.: Characterization of Mg0.5Zr2(PO4) 3 for potential use as an electrolyte in solid state magnesium batteries. Ceram Int. 40, 13719–13727 (2014)CrossRefGoogle Scholar
  18. 18.
    Vijayan, L., Govindaraj, G.: Structural and electrical properties of high-energy ball-milled NASICON type Li1.3Ti1.7Al0.3(PO4)2.9(VO4)0.1 ceramics. J Phys Chem Solids. 72, 613–619 (2011)CrossRefGoogle Scholar
  19. 19.
    Mariappan, C.R., Go, G.: Ac conductivity, dielectric studies and conductivity scaling of NASICON materials. Mater Sci Eng B. 94, 82–88 (2002)CrossRefGoogle Scholar
  20. 20.
    Almond, D.P.: Mobile ion concentrations in solid electrolytes from an analysis of a.c. conductivity. Solid State Ionics. 10, 277–282 (1983)CrossRefGoogle Scholar
  21. 21.
    Chowdari, B.V., Radhakrishnan, K., Thomas, K.A., Rao, G.S.: Ionic conductivity studies on Li1− xM2− xM′xP3O12 (H= Hf, Zr; M′= Ti, Nb). Mater Res Bull. 24, 221–229 (1989)CrossRefGoogle Scholar
  22. 22.
    Mouahid, F.E., Zahir, M., Maldonado-manso, P., Bruque, S., Losilla, E.R., Chimie, D., Doukkali, C., Jadid, E.: NASICON series: a Rietveld and impedance study. J Mater Chem. 3, 3258–3263 (2001)CrossRefGoogle Scholar
  23. 23.
    Mariappan, C.R., Govindaraj, G., Rathan, S.V., Prakash, G.V.: Preparation, characterization, ac conductivity and permittivity studies on vitreous M4AlCdP3 O12 ( M = Li, Na, K) system. Mater Sci Eng B. 121, 2–8 (2005)CrossRefGoogle Scholar
  24. 24.
    Ahmed, R., Moslehuddin, A.S.M., Mahmood, Z.H., Hossain, A.K.M.A.: Weak ferromagnetism and temperature dependent dielectric properties of Zn0.9Ni0.1O diluted magnetic semiconductor. Mater Res Bull. 63, 32–40 (2015)CrossRefGoogle Scholar
  25. 25.
    Subramanian, M. A., Subramanian, R., & Clearfield, A. Lithium ion conductors in the system AB (IV) 2 (PO4) 3 (B= Ti, Zr and Hf). Solid State Ionics, 18, 562-569 (1986)Google Scholar
  26. 26.
    Tan, F.K., Hassan, J., Wahab, Z.A.: Electrical conductivity and dielectric behavior of manganese and vanadium mixed oxide prepared by conventional solid state method. Engineering Science and Technology, an International Journal. 19(4), 2081–2087 (2016)CrossRefGoogle Scholar

Copyright information

© Australian Ceramic Society 2017

Authors and Affiliations

  1. 1.Department of Physics, Faculty of ScienceUniversiti Putra MalaysiaSerdangMalaysia
  2. 2.Institute of Advanced Technology (ITMA)Universiti Putra MalaysiaSerdangMalaysia
  3. 3.Department of Physics, Faculty of ScienceAhmadu Bello University ZariaKadunaNigeria

Personalised recommendations