Publication date: 10th April 2024
Development of new oxide ion conductor is important subject [1-3]. Recently new bismuth containing phases such as Dion-Jacobson phase CsBi2Ti2NbO10-δ or Sillén-Aurivillius phase, Bi3.9Sr0.1NbO8-δCl were reported as new oxide-ion conductors reaching log(σ /S∙cm-1) = 8.9 10-2 at1174 K and log(σ /S∙cm-1) = 2.99 10-2 at 873 K, respectively [1-2]. It was previously reported that the halide layer in the bismuth niobium oxychloride has a positive stabilizing effect and increases the stability of the material [1]. In this study, the conductivity of PbBiO2Cl, Sillén phase, a layered oxychloride material, explore substitution possibilities of Pb and Bi in the (PbBiO2)+ layer with iso- and aliovalent cations for increasing the oxide ion conductivity through introduction of interstitial oxygen or oxygen vacancies were measured.
Various cation doped PbBiO2Cl were successfully prepared and substitution of bismuth with an alkaline earth and an isovalent cation simultaneously (Ca2+ and Ga3+) is the most effective for increasing the conductivity and stability of PbBiO2Cl. The optimized dopant values were found to be 25mol% Ca and 10mol% Ga, PbBi0.65Ca0.25Ga0.1O2Cl. From electromotive force on O2-N2 cell and DC-polarisation measurements, oxide ion is not the major conducting spices which is estimated to be 20% or less of the total observed conduction, but the chlorine ion seems to be major charge carrier of which transport number is estimated to be higher than 40%. Consequently, this study reveals that doped PbBiO2Cl is a mixed anion conductor of Cl- and oxide ion, and small hole conduction. The oxide ion and Cl- conduction may occur in the bismuth-oxide [Bi2O2]2+ or [PbBiO2]+ layers and Cl layer in the Sillén and Sillén-Aurivillius structure, respectively.
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