Complex diffusion behavior of oxygen in nanocrystalline BaTiO3 ceramics

被引:17
作者
De Souza, Roger A. [1 ,2 ]
Voisin, Christophe [3 ]
Schraknepper, Henning [1 ,2 ]
Teusner, Markus [1 ,2 ]
Kessel, Markus [1 ,2 ]
Dufour, Pascal [3 ]
Tenailleau, Christophe [3 ]
Guillemet-Fritsch, Sophie [3 ]
机构
[1] Rhein Westfal TH Aachen, Inst Phys Chem, D-52056 Aachen, Germany
[2] JARA FIT, D-52056 Aachen, Germany
[3] Univ Toulouse 3, CNRS UMR 5085, Inst Carnot CIRIMAT, F-31062 Toulouse 9, France
关键词
DIELECTRIC-PROPERTIES; DEFECT CHEMISTRY; ION MIGRATION; PERMITTIVITY; KINETICS; EXCHANGE; SURFACE; OXIDE; ZR;
D O I
10.1039/c3cp53979b
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
O-18/O-16 exchange annealing and subsequent Time-of-Flight Secondary Ion Mass Spectrometry (ToF-SIMS) analysis is used to investigate oxygen transport in dense, nanocrystalline (average grain size d approximate to 300 nm) ceramics of nominally un-doped BaTiO3. Isotope penetration profiles are obtained as a function of temperature, 973 < T/K < 1173, at an oxygen activity aO(2) = 0.20 and as a function of oxygen activity, 0.002 < aO(2) < 0.20, at T = 1073 K. All isotope profiles show the same unusual shape: a flattened profile over the first similar to 10(2) nm, followed by a short, conventional diffusion profile. We demonstrate that the entire isotope profile can be described quantitatively by a numerical solution to the diffusion equation based on an increase in the local oxygen diffusion coefficient close to the surface. This position-dependent increase is attributed to additional oxygen vacancies that are generated by diffusion of chlorine impurities out of the ceramics. The presence of chlorine derives from the chemical route necessary to produce nanometric powders: it thus indicates a new manner in which nanocrystalline ceramics may differ from their microcrystalline counterparts.
引用
收藏
页码:2568 / 2575
页数:8
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