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从丰富的材料中获取高性能的热电材料:通过第二相纳米结构提高 PbS 的优值系数。

High performance thermoelectrics from earth-abundant materials: enhanced figure of merit in PbS by second phase nanostructures.

机构信息

Department of Chemistry, Northwestern University, Evanston, Illinois 60208, USA.

出版信息

J Am Chem Soc. 2011 Dec 21;133(50):20476-87. doi: 10.1021/ja208658w. Epub 2011 Nov 29.

Abstract

Lead sulfide, a compound consisting of elements with high natural abundance, can be converted into an excellent thermoelectric material. We report extensive doping studies, which show that the power factor maximum for pure n-type PbS can be raised substantially to ~12 μW cm(-1) K(-2) at >723 K using 1.0 mol % PbCl(2) as the electron donor dopant. We also report that the lattice thermal conductivity of PbS can be greatly reduced by adding selected metal sulfide phases. The thermal conductivity at 723 K can be reduced by ~50%, 52%, 30%, and 42% through introduction of up to 5.0 mol % Bi(2)S(3), Sb(2)S(3), SrS, and CaS, respectively. These phases form as nanoscale precipitates in the PbS matrix, as confirmed by transmission electron microscopy (TEM), and the experimental results show that they cause huge phonon scattering. As a consequence of this nanostructuring, ZT values as high as 0.8 and 0.78 at 723 K can be obtained for nominal bulk PbS material. When processed with spark plasma sintering, PbS samples with 1.0 mol % Bi(2)S(3) dispersion phase and doped with 1.0 mol % PbCl(2) show even lower levels of lattice thermal conductivity and further enhanced ZT values of 1.1 at 923 K. The promising thermoelectric properties promote PbS as a robust alternative to PbTe and other thermoelectric materials.

摘要

硫化铅是一种由高丰度元素组成的化合物,可以转化为一种优秀的热电材料。我们报告了广泛的掺杂研究,结果表明,使用 1.0 摩尔%的 PbCl2 作为电子施主掺杂剂,纯 n 型 PbS 的最大功率因子最大值可以在>723 K 时显著提高到~12 μW cm-1 K-2。我们还报告说,通过添加选定的金属硫化物相,可以大大降低 PbS 的晶格热导率。在 723 K 时,通过引入高达 5.0 摩尔%的 Bi2S3、Sb2S3、SrS 和 CaS,热导率可以分别降低约 50%、52%、30%和 42%。这些相在 PbS 基体中形成纳米级沉淀物,这通过透射电子显微镜(TEM)得到证实,实验结果表明它们会引起巨大的声子散射。由于这种纳米结构,名义块状 PbS 材料在 723 K 时可以获得高达 0.8 和 0.78 的 ZT 值。当用火花等离子体烧结处理时,PbS 样品中含有 1.0 摩尔%的 Bi2S3 分散相和掺杂 1.0 摩尔%的 PbCl2,显示出更低的晶格热导率,在 923 K 时进一步增强的 ZT 值为 1.1。有前途的热电性能使 PbS 成为 PbTe 和其他热电材料的可靠替代品。

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