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Insights into B-Site Ordering in Double Perovskite-Type Ba 3 Ca 1+ x Nb 2- x O 9-δ (0 ≤ x ≤ 0.45): Combined Synchrotron and Neutron Diffraction and Electrical Transport Analyses.
Inorganic Chemistry 2018 March 6
Perovskite-type metal oxides are being used in a wide range of technologies, including fuel cells, batteries, electrolyzers, dielectric capacitors, and sensors. One of their remarkable structural properties is cationic ordering in A or B sites, which affects electrical transport properties under different gaseous atmospheres, and chemical stability under CO2 and humid conditions. For example, a simple-perovskite-type Y-doped BaCeO3 forms BaCO3 and ((Ce,Y)O2-δ ) under CO2 at elevated temperature, while B-site-ordered double-perovskite-type Ba3 Ca1.18 Nb1.82 O9-δ remains chemically stable under the same conditions. Early structural studies on Ba3 Ca1+ x Nb2- x O9-δ (BCN) showed that the B-site ordering (1:1) is sensitive to the Ca content. However, ambiguity rises, as 1:2 B-site ordering was not observed in the parent and doped analogues when x was varied, which motivated us to revisit the complex oxides BCN ( x = 0-0.45) to determine the atomic structure by a mean of combined synchrotron X-ray and neutron diffraction methods. Surprisingly, the B-site ordering increases with increasing Ca/Nb mixing in the B-sites in BCN. In addition, the electrical conductivity of BCN was found to be the highest at x = ∼0.18, and it decreased as the Ca/Nb ratio further increased in BCN. Such a result was very similar to that for the Y-doped BaZrO3 , where the mobility of proton carriers was found to decrease as the dopant (Y) increased. A higher Ca/Nb ratio also promotes the growth of grain size, as Ca ions could serve as a sintering aid, improving the structural integrity.
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