中国物理B ›› 2009, Vol. 18 ›› Issue (7): 3084-3089.doi: 10.1088/1674-1056/18/7/079

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Synthesis and high temperature thermoelectric transport properties of Si-based type-I clathrates

唐润生1, 邓书康2, 唐新峰3   

  1. (1)Education Ministry Key Laboratory of Renewable Energy Advanced Materials and Manufacturing Technology; Yunnan Normal University, Kunming 650092, China; (2)Education Ministry Key Laboratory of Renewable Energy Advanced Materials and Manufacturing Technology; Yunnan Normal University, Kunming 650092, China;State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China; (3)State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
  • 收稿日期:2008-09-05 修回日期:2008-11-20 出版日期:2009-07-20 发布日期:2009-07-20
  • 基金资助:
    Project supported by the National Basic Research Program of China (Grant Nos 2007CB607501 and 2007CB607503) and Yunnan Natural Science Fund (Grant No 2008CD114).

Synthesis and high temperature thermoelectric transport properties of Si-based type-I clathrates

Deng Shu-Kang(邓书康)a)b)†, Tang Xin-Feng(唐新峰)b), and Tang Run-Sheng(唐润生)a)   

  1. a Education Ministry Key Laboratory of Renewable Energy Advanced Materials and Manufacturing Technology; Yunnan Normal University, Kunming 650092, China; b State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
  • Received:2008-09-05 Revised:2008-11-20 Online:2009-07-20 Published:2009-07-20
  • Supported by:
    Project supported by the National Basic Research Program of China (Grant Nos 2007CB607501 and 2007CB607503) and Yunnan Natural Science Fund (Grant No 2008CD114).

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摘要： N-type Si-based type-I clathrates with different Ga content were synthesized by combining the solid-state reaction method, melting method and spark plasma sintering (SPS) method. The effects of Ga composition on high temperature thermoelectric transport properties were investigated. The results show that at room temperature, the carrier concentration decreases, while the carrier mobility increases slightly with increasing Ga content. The Seebeck coefficient increases with increasing Ga content. Among all the samples, Ba7.93Ga17.13Si28.72 exhibits higher Seebeck coefficient than the others and reaches -135~μ V.K-1 at 1000 K. The sample prepared by this method exhibits very high electrical conductivity, and reaches 1.95× 105S.m-1 for Ba8.01Ga16.61Si28.93 at room temperature. The thermal conductivity of all samples is almost temperature independent in the temperature range of 300--1000~K, indicating the behaviour of a typical metal. The maximum {ZT} value of 0.75 is obtained at 1000~K for the compound Ba7.93Ga17.13Si28.72.

Abstract: N-type Si-based type-I clathrates with different Ga content were synthesized by combining the solid-state reaction method, melting method and spark plasma sintering (SPS) method. The effects of Ga composition on high temperature thermoelectric transport properties were investigated. The results show that at room temperature, the carrier concentration decreases, while the carrier mobility increases slightly with increasing Ga content. The Seebeck coefficient increases with increasing Ga content. Among all the samples, Ba7.93Ga17.13Si28.72 exhibits higher Seebeck coefficient than the others and reaches -135 μV$\cdot$K-1 at 1000 K. The sample prepared by this method exhibits very high electrical conductivity, and reaches 1.95×105S$\cdot$m-1 for Ba8.01Ga16.61Si28.93 at room temperature. The thermal conductivity of all samples is almost temperature independent in the temperature range of 300--1000 K, indicating the behaviour of a typical metal. The maximum ZT value of 0.75 is obtained at 1000 K for the compound Ba7.93Ga17.13Si28.72.

Key words: type-I clathrate, thermoelectric materials, synthesis

中图分类号:  (Metals, semimetals, and alloys)

  • 81.05.Bx
81.20.Ev (Powder processing: powder metallurgy, compaction, sintering, mechanical alloying, and granulation) 72.15.Jf (Thermoelectric and thermomagnetic effects) 72.15.Eb (Electrical and thermal conduction in crystalline metals and alloys)