A microcontact impedance study on NASICON-type Li1+xAlxTi2-x(PO4)3 (0 ≤ x ≤ 0.5) single crystals

D. Rettenwander, A. Welzl, S. Pristat, F. Tietz, S. Taibl, G. J. Redhammer, J. Fleig

Research output: Contribution to journalArticleResearchpeer-review

Abstract

We successfully demonstrated the applicability of microcontact impedance spectroscopy (MC IS) on Li+ conducting solid electrolytes and measured the Li+ bulk conductivity (σb) of LiTi2(PO4)3 (LTP) and Li1+xAlxTi2-x(PO4)3 (LATP) single crystals independent of microstructural effects (e.g., grain boundaries, pores, and density). The crystals had a size of about 100 μm in each direction and crystallized with NASICON-type structure (R3¯c). Finite element calculations were performed to validate the impedance data analysis. A strong increase in σb in the order of three magnitudes (3.16 × 10-6 to 1.73 × 10-3 S cm-1) was found after incorporating 0.1 mol Al3+ per formula unit into LTP. Moreover, since the crystal structural changes are almost linear in the LATP system up to x = 0.5, the increase of σb is most probably related to additional Li+ sites at the M3 (36f) position. The additional Li+ leads to a displacement of Li+ occupying the M1 (6b) sites towards the nearest-neighboring M3 position, and therefore opens the fast-conducting pathway within the NASICON structure. A significant change in σb was also observed as the Al3+ content further increased (x = 0.1 to 0.5). The highest σb value of 5.63 × 10-3 S cm-1 was obtained for samples with x = 0.4.

Original languageEnglish
Pages (from-to)1506-1513
Number of pages8
JournalJournal of materials chemistry / A
Volume4
Issue number4
DOIs
Publication statusPublished - 17 Dec 2015
Externally publishedYes

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Single crystals
Crystals
Solid electrolytes
Grain boundaries
Spectroscopy
Direction compound

ASJC Scopus subject areas

  • Chemistry(all)
  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

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A microcontact impedance study on NASICON-type Li1+xAlxTi2-x(PO4)3 (0 ≤ x ≤ 0.5) single crystals. / Rettenwander, D.; Welzl, A.; Pristat, S.; Tietz, F.; Taibl, S.; Redhammer, G. J.; Fleig, J.

In: Journal of materials chemistry / A, Vol. 4, No. 4, 17.12.2015, p. 1506-1513.

Research output: Contribution to journalArticleResearchpeer-review

Rettenwander, D. ; Welzl, A. ; Pristat, S. ; Tietz, F. ; Taibl, S. ; Redhammer, G. J. ; Fleig, J. / A microcontact impedance study on NASICON-type Li1+xAlxTi2-x(PO4)3 (0 ≤ x ≤ 0.5) single crystals. In: Journal of materials chemistry / A. 2015 ; Vol. 4, No. 4. pp. 1506-1513.
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abstract = "We successfully demonstrated the applicability of microcontact impedance spectroscopy (MC IS) on Li+ conducting solid electrolytes and measured the Li+ bulk conductivity (σb) of LiTi2(PO4)3 (LTP) and Li1+xAlxTi2-x(PO4)3 (LATP) single crystals independent of microstructural effects (e.g., grain boundaries, pores, and density). The crystals had a size of about 100 μm in each direction and crystallized with NASICON-type structure (R3¯c). Finite element calculations were performed to validate the impedance data analysis. A strong increase in σb in the order of three magnitudes (3.16 × 10-6 to 1.73 × 10-3 S cm-1) was found after incorporating 0.1 mol Al3+ per formula unit into LTP. Moreover, since the crystal structural changes are almost linear in the LATP system up to x = 0.5, the increase of σb is most probably related to additional Li+ sites at the M3 (36f) position. The additional Li+ leads to a displacement of Li+ occupying the M1 (6b) sites towards the nearest-neighboring M3 position, and therefore opens the fast-conducting pathway within the NASICON structure. A significant change in σb was also observed as the Al3+ content further increased (x = 0.1 to 0.5). The highest σb value of 5.63 × 10-3 S cm-1 was obtained for samples with x = 0.4.",
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