Asian Ceramic Science for Electronics III and Electroceramics in Japan XII

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Authors: Kenichi Kakimoto, Tatsuro Hotta, Hitoshi Ohsato
Abstract: Structural characterization of various (Li,Na,K)NbO3 solid solutions with different Li contents has been carried out by temperature-variable Raman scattering measurement. It was found that there was no clear thermal hysteresis between orthorhombic-tetragonal phase transition in the heating/cooling processes for (Li,Na,K)NbO3 ceramics with Li content of 6 wt% and above, although a noticeable thermal hysteresis is observed in the Raman spectra and dielectric constant measurement for the other specimens with lower Li contents. It is presumed that the structural change of (Li,Na,K)NbO3 cell tends to become insensibility against temperature as the Li content increases above 6.0 mol%.
Authors: Hitoshi Matsudo, Kenichi Kakimoto, Isao Kagomiya
Abstract: Na0.5K0.5NbO3 (NKN) lead-free piezoceramics was synthesized by a solid state reaction method. The d.c. conductivitydc and a.c. impedance of the ceramics were measured at the temperature range from 550 oC to room temperature on cooling process. Thedc decreased linearly with decreasing temperature on Arrhenius plot, and the activation energy at the temperature range from 450 to 390 oC and from 390 to 160 oC were 0.65 and 0.90 eV, respectively. The slope change at 390 oC corresponded to Curie temperature of NKN ceramics so that the carriers of these thermally active conductions were alkali metal or oxygen ions in the NKN crystal structure. The impedance of NKN ceramics at high temperature showed two relaxation processes at high and low frequencies, and the leak current was mainly attributed by the conduction through the grain boundary with low impedance value on lower frequency relaxation.
Authors: Satoshi Wada, Petr Pulpan
Abstract: Grain-oriented barium titanate (BaTiO3, BT) ceramics were prepared by a templated grain growth (TGG) method using [110]-oriented BT platelike particles as a template and hydrothermal BT sphere particles with different particle sizes as a matrix. The degree of orientation along the [110] direction, F110, was measured using an X-ray diffraction (XRD) pattern by the Lotgering method. To obtain both a high density and a high F110, the preparation conditions were optimized as functions of matrix particle size, volume fraction of the template to the matrix, and sintering temperature. As for the results, BT grain-oriented ceramics with a high density of more than 96 % were successfully prepared despite various F110 values from 0 to 98 %. Scanning electron microscopy (SEM) revealed that their average grain sizes were always 75 µm despite various F110 values and there were no anisotropic microstructures. These grain-oriented BT ceramics were poled at 100 °C, and their piezoelectric constants d33 was measured. As for the results, the d33 values increased with increasing F110 values, and at around an F110 of 85 %, d33 reached a maximum of 788 pC/N.
Authors: Chao Chen, Xiang Yong Zhao, Hong Liu, Wen Wei Ge, Hao Su Luo, Xiang Ping Jiang
Abstract: (1-x)(Na0.5Bi0.5)TiO3-xBaTiO3 (abbreviated as NBBT100(1-x)/100x or NBBT100x) solid solution single crystals with x=0, 0.06, 0.08, 0.10, 0.20, 1.0 were grown using top-seeded solution growth (TSSG) method. Dielectric, piezoelectric and ferroelectric properties of NBBT crystals were investigated as a function of temperature, frequency, composition and crystal orientation. The temperature (Tm) corresponding to dielectric maximum and the depolarization temperature (Td) decrease with increasing x. The <001> oriented NBBT90/10 single crystal shows excellent piezoelectric performance with piezoelectric constant (d33) value about 275pC/N and exhibits relatively smaller coercive field (Ec) of 2.49 kV/mm and dielectric loss tanδ of 2.9 %, indicating a more adaptive engineered domain structure.
Authors: Hiroyuki Shimizu, Yutaka Doshida, Satoshi Tanaka, Keizo Uematsu
Abstract: Recently, we have developed crystal-oriented sheet forming (COSF) process from green sheet process and high-magnetic-field method. We formed c-axis-oriented (Sr,Ca)2NaNb5O15 (SCNN) sheets by the COSF process, and succeeded in realizing c-axis-oriented single-plate type piezoelectric ceramics (O-SP) and c-axis-oriented multilayered type piezoelectric ceramics (O-MLPC) for SCNN. From the measurement results of displacement induced by electric field, it was clarified that effective d33 of the O-SP was 210~240 pm/V. This value was about 3 times larger than that of the randomly oriented single-plate type, which was 70% of that of single crystal. Moreover, it was confirmed that O-MLPC indicated displacements 2.5 times as large as that of the conventional multilayer piezoelectric ceramics. In this study, we clarified that piezoelectric properties in bulk and multilayer structure can be drastically enhanced using the COSF process.
Authors: Yuichi Sakai, Tomoaki Futakuchi, Masatoshi Adachi
Abstract: In order to prepare lead free multi-layer ceramic (MLC) actuators with Ni inner electrodes, inkjet ink containing NiO was prepared and its rheological properties were examined. The viscosity of the ink followed the Andrade's equation. By using this ink, Ba(Ti,Zr)O3 based MLCs were prepared. The printed NiO layers were reduced to metal Ni and they functioned as the inner electrodes. The remanent polarization of the MLCs increased with the grain growth caused by the increase of firing temperature. The remanent polarization Pr and coercive field Ec of the MLCs fired at 1400°C were 6.4 μC/cm2 and 3.5 kV/cm, respectively. The displacement of the MLCs with 7 active layers was approximately 320nm at 30 kV/cm. The effective d33 shows approximately 160 pm/V when the electric field was 10 kV/cm.
Authors: Yasuhiro Yoneda, Hiroyuki Saitoh, Kenji Yoshii, Takashi Nishida, Hironori Hayakawa, Naoshi Ikeda
Abstract: A new oxide, Bi(Mg1/2Ti1/2)O3 was prepared using a high-pressure high-temperature technique at 8 GPa and 1000°C. As-sintered Bi(Mg1/2Ti1/2)O3 has the BiFeO3-type perovskite structure with the rhombohedral R3c. After ground, crystal structure changed to tetragonal P4mm. Structure parameters of tetragonal Bi(Mg1/2Ti1/2)O3 were refined from laboratory X-ray powder diffraction data (a = 4.033(10) Å, and c = 3.938(10) Å). Bi(Mg1/2Ti1/2)O3 does not decompress at ambient pressure, but the structure changed from rhombohedral to tetragonal on heating above 800°C. This phase transition was nonreversible. Bi(Mg1/2Ti1/2)O3 is expected to be one of the end members of lead-free ferroelectric materials.
Authors: Satoshi Wada, Momoyo Nitta, Nobuhiro Kumada, Daisuke Tanaka, Masahito Furakawa, Chikako Moriyoshi, Yoshihiro Kuroiwa
Abstract: Barium titanate (BaTiO3, BT) and potassium niobate (KNbO3, KN) ceramics were prepared by normal sintering process. Phase diagram of BT-KN system was investigated using high-temperature XRD and dielectric measurement, and two phases coexistence between tetragonal and orthorhombic was observed at room temperature. Transmission electron microscope (TEM) observation confirmed that the microstructure of the ceramics with KN contents below 30 molar% was composed of only tetragonal BT-rich grain, while those with KN contents above 40 molar% were composed of two kinds of grains, i.e., tetragonal BT-rich and orthorhombic KN-rich grains. Phase boundary between two phases for BT-KN ceramics was grain boundary. Thus, we named two phases coexistence region for BT-KN ceramics “wide-band morphotropic phase boundary (MPB)”. Finally, dielectric and piezoelectric properties were investigated, and both dielectric and apparent d33 maximum were observed at the 0.5BT-0.5KN ceramics.
Authors: Keisuke Yamato, Nobuhiro Kumada, Chikako Moriyoshi, Yoshihiro Kuroiwa, Bong Yeon Lee, Takashi Iijima, Satoshi Wada
Abstract: Barium titanate (BaTiO3, BT) – bismuth lanthanum zinc titanium oxide [(BiyLa1-y)(Zn0.5Ti0.5)O3, ByL1-yZT] solid solution ceramics were prepared to enhance Curie temperature (TC) of BT, 132 °C, to 200 °C. As the raw materials, nanoparticles were used to make sintering temperatures lower. Optimization of calcination and sintering conditions resulted in a formation of a perovskite single-phase, and their densities were always greater than 94 %. The synchrotron XRD measurement revealed that the crystal structures were assigned to rhombohedral 3m. Temperature dependence of dielectric property revealed that for the 0.5BT-0.5BZT ceramics, TC was 230 °C. Moreover, La-doping into BT-BZT ceramics resulted in decrease of TC significantly. Finally, their piezoelectric properties were measured by electric-field dependence of strain at room temperature, and for the 0.6BT-0.4BZT ceramics, the apparent d33 was measured at 250 pC/N.

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