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Thermoelectric properties of Ru and In substituted misfit-layered Ca_3Co_4O_9

机译:Ru和In取代错配层Ca_3Co_4O_9的热电性质

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摘要

As an approach to improve the thermoelectric properties of the polycrystalline Ca_3Co_4O_9 misfit-layered oxide, substitutions of Co~(2+...4+) with the heavier cations Ru~(3+/4+) and In~(3+) were tested. Polycrystalline samples Ca_3Co_(4-x)Ru_xO_9 and Ca_3Co_(4-x)In_xO_9 (0 <x < 0.21) were prepared via a solid-state-reaction route. For each sample the crystal structure was analyzed and a complete thermoelectric characterization was done within a temperature range of 300 K < T< 1125 K. Both substitution strategies resulted in a significant decrease of the thermal conductivity (k). For the In~(3+)-substituted samples the decrease of the Seebeck coefficient (a) balanced the k reduction so that no overall enhancement of the figure of merit (ZT) was found. The Ru~(3+/4+) substitution reduced the p-type carrier concentration and thus increases the electrical resistivity (p_(el)), while a became larger at low temperatures. Despite the reduction of the power factor, a small enhancement in ZT was observed in the case of x = 0.1 Ru substitution, due to the strong k reduction. Considering the observed preferred orientation of the Ru-substituted crystallites, a maximum value of ZT = 0.14 perpendicular to the pressing direction is found at T = 1125 K, indicating that Ru substitution is a promising strategy for a further ZT improvement.
机译:作为改善多晶Ca_3Co_4O_9失配层氧化物热电性能的一种方法,用较重的阳离子Ru〜(3 + / 4 +)和In〜(3+)代替Co〜(2 + ... 4+)经过测试。通过固态反应路线制备了多晶样品Ca_3Co_(4-x)Ru_xO_9和Ca_3Co_(4-x)In_xO_9(0 <x <0.21)。对每个样品的晶体结构进行了分析,并在300 K <T <1125 K的温度范围内进行了完整的热电表征。两种替代策略均导致导热系数(k)大大降低。对于In〜(3+)取代的样品,塞贝克系数(a)的降低平衡了k的降低,因此未发现品质因数(ZT)的总体提高。 Ru〜(3 + / 4 +)取代降低了p型载流子浓度,从而增加了电阻率(p_(el)),而低温下a变大。尽管降低了功率因数,但由于x的强烈降低,在x = 0.1 Ru取代的情况下,ZT的增加很小。考虑到观察到的Ru-取代的微晶的优选取向,在T = 1125K处发现垂直于压制方向的ZT = 0.14的最大值,表明Ru取代是进一步改善ZT的有希望的策略。

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    Empa - Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Solid State Chemistry and Catalysis, UEberlandstr. 129, CH-8600 Duebendorf, Switzerland;

    Empa - Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Solid State Chemistry and Catalysis, UEberlandstr. 129, CH-8600 Duebendorf, Switzerland;

    Empa - Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Solid State Chemistry and Catalysis, UEberlandstr. 129, CH-8600 Duebendorf, Switzerland;

    Empa - Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Solid State Chemistry and Catalysis, UEberlandstr. 129, CH-8600 Duebendorf, Switzerland;

    University of Berne, Department of Chemistry and Biochemistry, CH-3012 Berne, Switzerland;

    Empa - Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Solid State Chemistry and Catalysis, UEberlandstr. 129, CH-8600 Duebendorf, Switzerland;

    Empa - Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Solid State Chemistry and Catalysis, UEberlandstr. 129, CH-8600 Duebendorf, Switzerland,University of Berne, Department of Chemistry and Biochemistry, CH-3012 Berne, Switzerland;

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