Journal
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
Volume 22, Issue 3, Pages 727-737Publisher
SPRINGER
DOI: 10.1007/s10008-017-3797-7
Keywords
Mixed conductors; Si-doping; Strontium ferrite; Domain structure; Oxygen nonstoichiometry; Defect equilibria; Electron mobility
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Funding
- Russian Foundation for Basic Research [17-08-01029]
- Ministry of Education and Science of the Russian Federation [14.B25.31.0018]
- Russian Science Foundation [17-79-30071]
- FCT, Portugal [UID/EMS/00481/2013, UID/Multi/04349/2013]
- FEDER, Portugal [CENTRO-01-0145-FEDER-022083]
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Oxygen nonstoichiometry of perovskite-like SrFe1-x Si (x) O3-delta (x = 0.05-0.20), studied by thermogravimetric analysis and coulometric titration in the oxygen partial pressure range 10(-20)-0.5 atm at 700-950 A degrees C, decreases with Si4+ additions. The equilibrium -T-delta diagrams can be adequately described by a model accounting for anion site-exclusion effects near highly stable SiO4 tetrahedra and energetic favorability of the defect clusters formed by two tetrahedra sharing one oxygen vacancy. This model was validated by atomistic computer simulations. The standard thermodynamic functions for oxygen incorporation and iron disproportionation reactions are essentially independent of silicon concentration, as for the migration activation energies of the p- and n-type electronic charge carriers. On the contrary, at low temperatures, Si-doping leads to a higher oxygen deficiency, simultaneously suppressing long-range vacancy ordering and increasing oxygen coordination of iron cations as estimated from the Mossbauer spectra. These phenomena are associated, again, with vacancy trapping near randomly distributed Si4+. The Mossbauer spectroscopy, transmission electron microscopy, and electron diffraction studies showed that Si4+ substitution progressively reduces the content of brownmillerite-like nanodomains typical for SrFeO3-based materials.
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