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A7: Developments in measurement techniques and preparation methods

Hirofumi Kakemoto1, Takuto Kawano2, Kensuke Ozawa2, and Hiroshi Irie1,2
1Clean Energy Research Center, University of Yamanashi, 2Interdisciplinary Graduate School of Medicine and Engineering, University of Yamanashi

Thermoelectric (TE) property of NaxCoO2 (NCO, P-type) gives many impacts to develop oxide TE materials. Low thermal conductivity (κ) is found in oxide TE materials, and it favorable to increase dimension less figure of merit (ZT=S2σT/κ, S: Seebeck coefficient, σ:electrical conductivity). Although partly reduced Na (κNa>100 W/mK) layer involves in NCO, κ is possible to be decreased until 20 W/mK with conductive CoO2 layered crystal structure. Nb-doped SrTiO3 (STO, N-type) also shows excellent TE properties, on the other hand k of STO is slightly high vale (10 W/mK) with cubic structure. Tungsten bronze type oxide (TB) such as Sr1-xBaxNb2O6 (SBN) and Ba2NaNb5O15 (BNN) are well known for electro-optic crystal. N-type TE property of reduced SBN single crystal is firstly reported about typical S and σ for c-axis. As a function of oxygen reduction, total κtot (κtot=κph+κe) of reduced BNN is affected by decreasing κph and increasing κe. We evaluate κ of reduced BNN from theoretical evaluation and experimental study. In experimental, BNN was prepared from BaCO3, NaCl and Nb2O5 powders at 1100oC-1300oC for 12h by solid state reaction. Needle-like (Ba, Na)Nb2O6 (N-BNN) particles were synthesized at 900oC-1100oC for 4h in closed crucible. Mixture of BNN and N-BNN was made by tape casting for in-plane orientation, and was sintered at 1340oC for 12h. Orient BNN was partly reduced at 1050oC-1100oC for 2-5h in CO atmosphere. Temperature dependence of S and that of σ for reduced BNN were measured from 20oC to 300oC by conventional two probe method and four-terminal method, respectively. Curve fitting (follows Gasumyants’ eq.) was carried out for temperature dependence of S data. ZT and κ of BNN were measured by using Harman method. In presentation, we will report about κ of non-stoichiometric BNN utilizing Harman method for ZT. κ and comparison with theoretical evaluation (WIEN2K, BoltzTrap).