高填充量BaxEuyCo4Sb12方钴矿热电性能研究

doi:10.3724/SP.J.1077.2012.12615

摘要/Abstract

摘要：

利用熔融法和等离子放电烧结(SPS)制备单相双原子填充Ba_xEu_yCo₄Sb₁₂方钴矿材料并测试其高温热电性能。实验发现, 在高填充量下(x+y>40%), 材料在高温时具有高的功率因子(>60 W/(cm•K²))。在方钴矿的晶格空洞中同时引入Ba和Eu两种填充原子, 能增强晶格声子散射, 从而大幅降低方钴矿的晶格热导。实验证实, Ba_xEu_yCo₄Sb₁₂体系的晶格热导显著降低, 其室温晶格热导最低达1.7 W/(m•K)。与此对应的是双原子填充Ba_xEu_yCo₄Sb₁₂方钴矿材料的热电优值(ZT值)明显增大, 其中Ba_0.19Eu_0.23Co₄Sb₁₂的ZT值在850 K时达到了1.3。

关键词: 热电, 填充方钴矿, 输运性能

Abstract:

Filled skutterudite is one of the most promising thermoelectric materials for power generation applications. We report the high-temperature thermoelectric properties including electrical conductivity, Seebeck coefficient, and thermal conductivity in single-phased polycrystalline dual-element-filled skutterudites Ba_xEu_yCo₄Sb₁₂(0<x<0.2, 0<y<0.3). The double-filled skutterudites are synthesized by the melting-quenching-annealing method and the bulk pellects are sintered by spark plasma sintering (SPS). High total filling fractions (x+y>40%) with very large power factor of Ba_xEu_yCo₄Sb₁₂over 60 μW/(cm•K²) at high temperature is obtained. The combination of Ba and Eu fillers inside the voids of the skutterudite structure provides a broad range of resonant phonon scattering and consequently a strong suppression in the lattice thermal conductivity is observed. The lattice thermal conductivity values for Ba_xEu_yCo₄Sb₁₂system are dramatically decreased and the lowest value is about 1.7 W/(m•K) at room temperature. Consequently, enhanced thermoelectric figure of merits (ZT) for Ba and Eu dual-element-filled CoSb₃ skutterudites are obtained at elevated temperatures, in particular ZT=1.3 at 850 K for Ba_0.19Eu_0.23Co₄Sb₁₂.

Key words: thermoelectric, filled-skutterudite, transport properties

中图分类号:

TQ174

吴汀, 柏胜强, 史迅, 陈立东. 高填充量Ba_xEu_yCo₄Sb₁₂方钴矿热电性能研究[J]. 无机材料学报, 2013, 28(2): 224-228.

WU Ting, BAI Sheng-Qiang, SHI Xun, CHEN Li-Dong. Enhanced Thermoelectric Properties of Ba_xEu_yCo₄Sb₁₂ with Very High Filling Fraction[J]. Journal of Inorganic Materials, 2013, 28(2): 224-228.

图/表 6

Fig. 1 Measured temperature dependence of the electrical conductivity (σ) in double-filled skutterudites

Fig. 2 Measured temperature dependence of the Seebeck coefficient (S) in double-filled skutterudites

Fig. 3 Measured temperature dependence of the Seebeck coefficient (S2σ) in double-filled skutterudites

Fig. 4 Measured temperature dependence of total thermal conductivity (κ) in double-filled skutterudites

Fig. 5 Measured temperature dependence of lattice thermal conductivity (κL) in double-filled skutterudites

Fig. 6 Measured temperature dependence of dimensionless figure of merit (ZT) in double-filled skutterudites

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高填充量Ba_xEu_yCo₄Sb₁₂方钴矿热电性能研究

Enhanced Thermoelectric Properties of Ba_xEu_yCo₄Sb₁₂ with Very High Filling Fraction

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