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Journal of the Korean Physical Society

, Volume 69, Issue 5, pp 798–805 | Cite as

Thermoelectric properties of p-type partially double-filled (Pr1−z Nd z ) y Fe4−x Co x Sb12 skutterudites

  • Dong-Kil Shin
  • Il-Ho KimEmail author
Article

Abstract

p-Type partially double-filled (Pr1−z Nd z ) y Fe4−x Co x Sb12 (z = 0.25, 0.75, y = 0.8, 0.9, and x = 0, 0.5, 1.0) skutterudites were synthesized by encapsulated melting and annealing and consolidated by hot pressing. The effects of Pr/Nd partial double-filling and Co substitution for Fe (charge compensation) on the electronic transport and the thermoelectric properties of the skutterudites were examined. A few secondary phases such as marcasite FeSb2 were formed together with the skutterudite phase, but the formation was suppressed with increasing Co content. Unlike for complete filling with Pr/Nd, the (Pr,Nd)Sb2 phases were not formed by partial filling with Pr/Nd. Successful Pr/Nd double filling in the voids and Co substitution for Fe were confirmed because the lattice constant increased with increasing filling fraction and Pr/Nd ratio, and decreased with increasing Co content. The electrical conductivity slightly decreased with increasing temperature, showing degenerate semiconductor characteristics, while the Hall and the Seebeck coefficients showed positive signs, indicating that holes were the major carriers (p-type conductions). The Seebeck coefficient increased due to a decrease in the carrier concentration with increasing Pr and Co contents while the electrical conductivity decreased. The lattice thermal conductivity decreased because phonon scattering was enhanced by Pr and Nd double filling, which led to low thermal conductivity, but partially double-filled specimens did not have a significant effect on the reduction of lattice thermal conductivity compared with the completely double-filled specimens. The maximum dimensionless figure of merit, ZT = 0.84, was obtained at 723 K for (Pr0.75Nd0.25)0.8Fe3CoSb12.

Keywords

Thermoelectric Skutterudite Double filling Charge compensation 

PACS numbers

72.15.Jf 72.20.Pa 

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References

  1. [1]
    G. A. Slack, Handbook of Thermoelectrics, edited by D. M. Rowe (CRC, Boca Raton, FL, 1995), Chap. 34.Google Scholar
  2. [2]
    P. F. Qiu, J. Yang, R. H. Liu, X. Shi, X. Y. Huang, G. J. Snyder, W. Zhang and L. D. Chen, J. Appl. Phys. 109, 063713 (2011).ADSCrossRefGoogle Scholar
  3. [3]
    D. T. Morelli and G. P. Meisner, J. Appl. Phys. 77, 3777 (1995).ADSCrossRefGoogle Scholar
  4. [4]
    Q. Li, Z. W. Lin and J. Zhou, J. Electron. Mater. 38, 1268 (2009).ADSCrossRefGoogle Scholar
  5. [5]
    G. Rogl, A. Grytsiv, P. Rogl, E. Bauer and M. Zehetbauer, Intermet. 19, 546 (2010).CrossRefGoogle Scholar
  6. [6]
    G. S. Nolas, J. L. Cohn and G. A. Slack, Phys. Rev. B 58, 164 (1998).ADSCrossRefGoogle Scholar
  7. [7]
    G. S. Nolas, M. Kaeser, R. T. Littleton and T. M. Tritt, Appl. Phys. Lett. 77, 1855 (2000).ADSCrossRefGoogle Scholar
  8. [8]
    D. T. Morelli, G. P. Meisner, B. X. Chen, S. Q. Hu and C. Uher, Phys. Rev. B 56, 7376 (1997).ADSCrossRefGoogle Scholar
  9. [9]
    L. D. Chen, T. Kawahara, X. F. Tang, T. Goto, T. Hirai, J. S. Dyck, W. Chen and C. Uher, J. Appl. Phys. 90, 1864 (2001).ADSCrossRefGoogle Scholar
  10. [10]
    X. Shi et al., J. Am. Chem. Soc. 133, 7837 (2011).CrossRefGoogle Scholar
  11. [11]
    G. P. Meisner, D. T. Morelli, S. Hu, J. Yang and C. Uher, Phys. Rev. Lett. 80, 3551 (1998).ADSCrossRefGoogle Scholar
  12. [12]
    B. C. Sales, D. Mandrus and R. K. Williams, Science 272, 1325 (1996).ADSCrossRefGoogle Scholar
  13. [13]
    Z. Chen, J. O. Yang, R. H. Liu, L. L. Xi, W. Q. Zhang and J. Yang, J. Electron. Mater. 42, 2492 (2013).ADSCrossRefGoogle Scholar
  14. [14]
    J. Yang, W. Zhang, S. Q. Bai, Z. Mei and L. D. Chen, Appl. Phys. Lett. 90, 192111 (2007).ADSCrossRefGoogle Scholar
  15. [15]
    C. Uher, Thermoelectrics Handbook, edited by D. M. Rowe (CRC, Boca Raton, FL, 2006), Chap. 34.Google Scholar
  16. [16]
    X. Shi, S. Q. Bai, L. L. Xi, J. O. Yang, W. Q. Zhang, L. D. Chen and J. Yang, J. Mater. Res. 26, 1745 (2011).ADSCrossRefGoogle Scholar
  17. [17]
    R. H. Liu, J. O. Yang, X. H. Chen, X. Shi, L. D. Chen and C. Uher, Intermet. 19, 1747 (2011).CrossRefGoogle Scholar
  18. [18]
    W. Zhao, Q. Zhang, C. Dong, L. Liu and X. Tang, J. Am. Chem. Soc. 131, 3713 (2009).CrossRefGoogle Scholar
  19. [19]
    C. Uher, C. P. Li and S. Ballikaya, J. Electron. Mater. 39, 9 (2010).CrossRefGoogle Scholar
  20. [20]
    J. Graff, S. Zhu, T. Holgate, J. Peng, J. He and T. M. Tritt, J. Electron. Mater. 40, 5 (2011).CrossRefGoogle Scholar
  21. [21]
    G. Rogl et al., Acta Mater. 60, 2146 (2012).CrossRefGoogle Scholar
  22. [22]
    G. Rogl, A. Grytsiv, P. Rogl, N. Peranio, E. Bauer, M. Zehetbauer and O. Eibl, Acta Mater. 63, 30 (2014).CrossRefGoogle Scholar
  23. [23]
    L. Zhou, P. F. Qiu, C. Uher, X. Shi and L. D. Chen, Intermet. 32, 209 (2013).CrossRefGoogle Scholar
  24. [24]
    G. Rogl, A. Grytsiv, E. Bauer, P. Rogl and M. Zehetbauer, Intermet. 18, 57 (2010).CrossRefGoogle Scholar
  25. [25]
    G. Rogl, A. Grytsiv, M. Falmbigl, E. Bauer, P. Rogl, M. Zehetbauer and Y. Gelbstein, J. Alloys Compd. 537, 242 (2012).CrossRefGoogle Scholar
  26. [26]
    X. Meng, W. Cai, Z. Liu, J. Li, H. Geng and J. Sui, Acta Mater. 98, 405 (2015).CrossRefGoogle Scholar
  27. [27]
    D. K. Shin and I. H. Kim, J. Korean Phys. Soc. 66, 1879 (2015).ADSCrossRefGoogle Scholar
  28. [28]
    G. J. Tan, S. Y. Wang, Y. G. Yan, H. Li and X. F. Tang, J. Electron. Mater. 41, 1147 (2012).ADSCrossRefGoogle Scholar
  29. [29]
    Y. C. Lan, A. J. Minnich, G. Chen and Z. F. Ren, Adv. Funct. Mater. 20, 357 (2010).CrossRefGoogle Scholar
  30. [30]
    C. Kittel, Introduction to Solid State Physics, 6th ed. (Wiley, New York, 1986), p. 152.Google Scholar
  31. [31]
    G. J. Tan, S. Y. Wang and X. F. Tang, J. Electron. Mater. 43, 1712 (2014).ADSCrossRefGoogle Scholar

Copyright information

© The Korean Physical Society 2016

Authors and Affiliations

  1. 1.Department of Materials Science and EngineeringKorea National University of TransportationChungjuKorea

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