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Journal of Inorganic Materials

Journal of Inorganic Materials >

2013 , Vol. 28 >Issue 2: 224 - 228

DOI: https://doi.org/10.3724/SP.J.1077.2012.12615

Orginal Article

Enhanced Thermoelectric Properties of BaxEuyCo4Sb12 with Very High Filling Fraction

  • Ting WU ,
  • Sheng-Qiang BAI ,
  • Xun SHI ,
  • Li-Dong CHEN
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  • (CAS Key Laboratory of Energy-conversion Materials, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China)
吴 汀. E-mail: wuting@mail.sic.ac.cn

Received date: 2012-10-17

  Online published: 2013-01-23

Supported by

Foundation item: National Natural Science Foundation of China (51004096, 51102260)

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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 BaxEuyCo4Sb12(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 BaxEuyCo4Sb12 over 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 BaxEuyCo4Sb12 system 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 Ba0.19Eu0.23Co4Sb12.

Key words： thermoelectric; filled-skutterudite; transport properties

Cite this article

Ting WU , Sheng-Qiang BAI , Xun SHI , Li-Dong CHEN . Enhanced Thermoelectric Properties of BaxEuyCo4Sb12 with Very High Filling Fraction[J]. Journal of Inorganic Materials, 2013 , 28(2) : 224 -228 . DOI: 10.3724/SP.J.1077.2012.12615

References

[1] Slack G A. In: Rowe D M, editor. CRC Handbook of Thermoelectrics. Boca Raton, FL: CRC Press; 1995: 407.
[2] Sales B C, Mandrus D, Williams R K. Filled skutterudite antimonides: a
[2] new class of thermoelectric materials.Science, 1996, 272(5266):1325-1328.
[3] Sales B C, Mandrus D, Chakoumakos B C, et al. Filled skutterudite antimonides: electron crystals and phonon glasses. Phys. Rev. B, 1997, 56(23): 15081-15089.
[4] Nolas G S, Cohn J L, Slack G A. Effect of partial void filling on the lattice thermal conductivity of skutterudites. Phys. Rev. B, 1998, 58(1):164-170.
[5] Chen L D, Karahara T, Tang X F, et al. Anomalous barium filling fraction and n-type thermoelectric performance of BayCo4Sb12. J. Appl. Phy., 2001, 90(8):1864-1868.
[6] Zhao X Y, Shi X, Chen L D, et al. Synthesis and thermoelectric properties of Sr-filled skutterudite SryCo4Sb12. J. Appl. Phy. , 2006, 99(5): 053711-1-4.
[7] Puyet M, Lenoir B, Dauscher A, et al. High temperature transport properties of partially filled CaxCo4Sb12 skutterudites. J. Appl. Phy., 2004, 95(9): 4852-4855.
[8] Morelli D T, Meisner G P, Chen B X, et al. Cerium filling and doping of cobalt triantimonide. Phys. Rev. B, 1997, 56(12): 7376-7383.
[9] Nolas G S, Kaeser M, Littleton V R T, et al. High figure of merit in partially filled ytterbium skutterudite materials. Appl. Phys. Lett., 2000, 77(12):1855-1857.
[10] Lamberton G A, Bhattacharya S, Littleton R T, et al. High figure of merit in Eu-filled CoSb3-based skutterudites. Appl. Phys. Lett., 2002, 80(4): 598-600.
[11] Kuznetsov V L, Kuznetsov L A, Rowe D M. Effect of partial void filling on the transport properties of NdxCo4Sb12 skutterudites. J. Phys.: Condens. Matter, 2003, 15(29): 5035-5048.
[12] Pei Y Z, Chen L D, Zhang W, et al. Synthesis and thermoelectric properties of KyCo4Sb12. Appl. Phys. Lett. , 2006, 89(22): 221107-1-3.
[13] Pei Y Z, Yang J, Chen L D, et al. Improving thermoelectric performance of caged compounds through light-element filling. Appl. Phys. Lett. , 2009, 95(4): 042101-1-3.
[14] Sales B C, Chakoumakos B C, Mandrus D. Thermoelectric properties of thallium-filled skutterudites. Phys. Rev. B, 2000, 61(4): 2475-2481.
[15] Nolas G S, Takizawa H, Endo E, et al. Thermoelectric properties of Sn-filled skutterudites. Appl. Phys. Lett., 2000, 77(10): 52-54.
[16] Nolas G S, Yang J, Takizawa H. Transport properties of germanium-filled CoSb3. Appl. Phys. Lett., 2004, 84(25): 5210-5212.
[17] Uher C. In: Tritt T M, editor. Recent Trends in Thermoelectric Materials Research I, Semiconductors and Semimetals. CA: Academic Press, 2000:139.
[18] Yang J, Zhang W, Bai S Q, et al. Dual-frequency resonant phonon scattering in BaxRyCo4Sb12. Appl. Phys. Lett. , 2007, 90(19): 192111-1-3.
[19] Berardan D, Alleno E, Godart C, et al. Improved thermoelectric properties in double-filled Cey/2Yby/2Fe4-x(Co/Ni)xSb12 skutterudites. J. Appl. Phys. , 2005, 98(3):033710-1-6.
[20] Lu Q M, Zhang J X, Zhang X, et al. Effects of double filling of La and Ce on thermoelectric properties of CemLanFe1.0Co3.0Sb12 compounds by spark plasma sintering. J. Appl. Phys. , 2005, 98:106107-1-3.
[21] Tang X F, Li H, Zhang Q J, et al. Synthesis and thermoelectric properties of double-atom-filled skutterudite compounds CamCenFexCo4-xSb12. J. Appl. Phys. , 2006, 100(12): 123702-1-8.
[22] Bai S Q, Pei Y Z, Chen L D, et al. Enhanced thermoelectric performance of dual-element-filled skutterudite BaxCeyCo4Sb12. Acta Mater. Appl., 2009, 57(11): 3135-3139.
[23] Bai S Q, Shi X, Chen L D. Lattice thermal transport in BaxREyCo4Sb12(RE=Ce, Yb, and Eu) double-filled skutterudites. Appl. Phys. Lett. , 2010, 96(20): 202102-1-3.
[24] Shi X, Kong H, Uher C, et al. Low thermal conductivity and high thermoelectric figure of merit in n-type BaxYbyCo4Sb12 double- filled skutterudites. Appl. Phys. Lett. , 2008, 92(18): 182101-1-3.
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