Effects of Ba Deficiency on Ion Ordering, Grain Growth, and Microwave Dielectric Properties of Ba₁₋xZn₁/₃Nb₂/₃O₃ Ceramics

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<jats:p> Ba<jats:sub>1-<jats:italic>x</jats:italic> </jats:sub>Zn<jats:sub>1/3</jats:sub>Nb<jats:sub>2/3</jats:sub>O<jats:sub>3</jats:sub> (0≤<jats:italic>x</jats:italic>≤0.02) ceramics were prepared by the solid-state reaction. The effects of Ba deficiency on the long-range order (LRO) of B-site ions, grain growth, and microwave dielectric properties of Ba<jats:sub>1-<jats:italic>x</jats:italic> </jats:sub>Zn<jats:sub>1/3</jats:sub>Nb<jats:sub>2/3</jats:sub>O<jats:sub>3</jats:sub> ceramics were investigated. Results show that Ba deficiency can effectively improve the sinterability of the ceramics and reduce the densification temperature by about 100 °C. The X-ray diffraction (XRD) and Raman spectra reveal that Ba-deficient samples exhibit a higher degree of LRO, and that the samples with <jats:italic>x</jats:italic> = 0.01 exhibit the highest degree of LRO. Furthermore, the degree of LRO increases with the decrease in sintering temperature in the range of 1400–1550 °C. Good microwave dielectric properties of ε<jats:sub>r</jats:sub> = 39.8, <jats:italic>Q</jats:italic> ×<jats:italic>f</jats:italic> = 66532 GHz, and τ<jats:sub>f</jats:sub> = +23.9 ppm/°C are obtained for the Ba-deficient samples with <jats:italic>x</jats:italic> = 0.01 when sintered at 1450 °C for 4 h. After a second sintering process at 1400 °C/10 h during cooling, the <jats:italic>Q</jats:italic> ×<jats:italic>f</jats:italic> values of Ba<jats:sub>1-<jats:italic>x</jats:italic> </jats:sub>Zn<jats:sub>1/3</jats:sub>Nb<jats:sub>2/3</jats:sub>O<jats:sub>3</jats:sub> ceramics are improved. An optimized <jats:italic>Q</jats:italic> ×<jats:italic>f</jats:italic> value of 72650 GHz is obtained for the Ba<jats:sub>0.99</jats:sub>Zn<jats:sub>1/3</jats:sub>Nb<jats:sub>2/3</jats:sub>O<jats:sub>3</jats:sub> (<jats:italic>x</jats:italic> = 0.01) ceramics after two-step sintering. </jats:p>

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