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Proton and oxygen ion conductivity in the pyrochlore/fluorite family of Ln2-xCaxScMO7-δ (Ln = La, Sm, Ho, Yb; M= Nb, Ta; x = 0, 0.05, 0.1) niobates and tantalates

Abstract

The tolerance factor is a good criterion to understand the structural transitions in Ln2-xCaxScMO7-δ (Ln = La, Sm, Ho, Yb; M = Nb, Ta; x = 0, 0.05, 0.1). Decreasing the Ln ionic radius in Ln2ScNb(Ta)O7 leads to a morphotropic transition from the pyrochlore to a fluorite-like structure. The Ca2+- doping leads to a pyrochlore-to-fluorite transition in Ln2-xCaxScMO7-δ (Ln = La, Sm) and a fluorite-to-pyrochlore transition in Ho2-xCaxScNbO7-δ. Proton contribution to the total conductivity was observed for Ln2-xCaxScNb(Ta)O7 (Ln = La, Sm; x= 0, 0.05, 0.1) 3+/5 pyrochlores and maximum of proton contribution was shown by Sm1.9Ca0.1ScMO6.95 (M = Nb, Ta), which are located at the boundary between pyrochlores and fluorites (comparative study of electrical conduction and oxygen diffusion). Proton conduction of Sm1.9Ca0.1ScNbO6.95 and Sm1.9Ca0.1ScTaO6.95 pyrochlores persists up to 800 and 850 °C, respectively. The conductivity of fluorite-like Ho2-xCaxScNbO7 (x= 0, 0.05) and Yb2ScNbO7 is dominated by the oxygen ion transport, in accordance with their energy activation values 1.09-1.19 eV. The dielectric permittivity and TG studies were used for investigation of oxygen vacancies dynamics and water incorporation in Ln2-xCaxScNb(Ta)O7 (Ln = La, Sm, Ho, Yb; x= 0, 0.05, 0.1). It is shown that an oxygen vacancy-related dielectric relaxation in the range of 550–650 °C (ambient air), typical for pyrochlores and fluorites with pure oxygen ion conductivity, decreases and disappears for proton - conducting oxides.

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Publication details

The article was received on 17 Oct 2017, accepted on 12 Jan 2018 and first published on 12 Jan 2018


Article type: Paper
DOI: 10.1039/C7DT03912C
Citation: Dalton Trans., 2018, Accepted Manuscript
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    Proton and oxygen ion conductivity in the pyrochlore/fluorite family of Ln2-xCaxScMO7-δ (Ln = La, Sm, Ho, Yb; M= Nb, Ta; x = 0, 0.05, 0.1) niobates and tantalates

    A. V. Shlyakhtina, K. S. Pygalskiy, D. A. Belov, N. V. Lyskov, E. P. Kharitonova, I. V. Kolbanev, A. B. Boruniova, O. K. Karyagina, E. Sadovskaya, V. A. Sadykov and N. F. Eremeev, Dalton Trans., 2018, Accepted Manuscript , DOI: 10.1039/C7DT03912C

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