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三元假锰钡矿型 BaxCr5Se8(0.5 < x < 0.55)固溶体的磁性和热电性能

Magnetic and thermoelectric properties of the ternary pseudo-hollandite BaxCr5Se8 (0.5 < x < 0.55) solid solution.

作者信息

Lefèvre Robin, Berthebaud David, Bux Sabah, Hébert Sylvie, Gascoin Franck

机构信息

Laboratoire CRISMAT UMR 6508 CNRS ENSICAEN UCBN, 6 Boulevard du Maréchal Juin, 14050, Caen Cedex 04, France.

Jet Propulsion Laboratory, 4800 Oak Grove Drive MS: 277-207 Pasadena, CA 91109, USA.

出版信息

Dalton Trans. 2016 Jul 26;45(30):12119-26. doi: 10.1039/c6dt02166b.

Abstract

The structure of Ba0.5Cr5Se8 has been recently resolved, and its thermoelectric and magnetic properties have been studied. A ZT of 0.12 was found at around 800 K. Here, we report a study on the pseudo-hollandite BaxCr5Se8 solid-solution with 0.5 ≤ x ≤ 0.55 and its thermoelectric and magnetic properties. There is no significant impact either on the cell parameters depending on the cation content or on the magnetic properties. However, thermoelectric properties are radically changed depending on x content. While the low thermal conductivity, around 0.8 W m(-1) K(-1), remains similar for all samples, a respective increase and decrease of the resistivity and the Seebeck coefficient are observed with increasing Ba content. The maximum Seebeck coefficient is found with Ba0.5Cr5Se8 at around 635 K with 315 μV K(-1), and the Seebeck coefficient then decreases and is correlated with an activation of minority charge carriers confirmed by Hall measurements. A similar but steeper behavior is observed for the Ba0.55Cr5Se8 temperature dependence plot at around 573 K. Finally, the best thermoelectric performances are found using the lowest content of Ba, unlike when x tends to 0.55, ZT approaches a tenth of the initial best value. BaxCr5Se8 compounds are antiferromagnetic with TN = 58 K. A large peak in thermal conductivity is observed around the antiferromagnetic transition for all stoichiometry.

摘要

Ba0.5Cr5Se8的结构最近已得到解析,并对其热电和磁性能进行了研究。在800 K左右发现其热电优值(ZT)为0.12。在此,我们报道了对阳离子含量为0.5 ≤ x ≤ 0.55的假砷锰矿型BaxCr5Se8固溶体及其热电和磁性能的研究。阳离子含量对晶胞参数或磁性能均无显著影响。然而,热电性能随x含量的变化而发生显著改变。虽然所有样品的低热导率(约0.8 W m(-1) K(-1))保持相似,但随着Ba含量的增加,电阻率和塞贝克系数分别出现增加和减小。在Ba0.5Cr5Se8中,在约635 K时发现最大塞贝克系数为315 μV K(-1),随后塞贝克系数减小,这与霍尔测量证实的少数载流子的激活有关。在约573 K时,Ba0.55Cr5Se8的温度依赖性曲线呈现出类似但更陡峭的行为。最后,发现使用最低Ba含量时热电性能最佳,与x趋于0.55时不同,此时ZT接近初始最佳值的十分之一。BaxCr5Se8化合物为反铁磁性,奈尔温度(TN) = 58 K。对于所有化学计量比,在反铁磁转变附近均观察到热导率出现一个大的峰值。

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