Article | Published:

Strained endotaxial nanostructures with high thermoelectric figure of merit

Nature Chemistry volume 3, pages 160166 (2011) | Download Citation

Subjects

Abstract

Thermoelectric materials can directly generate electrical power from waste heat but the challenge is in designing efficient, stable and inexpensive systems. Nanostructuring in bulk materials dramatically reduces the thermal conductivity but simultaneously increases the charge carrier scattering, which has a detrimental effect on the carrier mobility. We have experimentally achieved concurrent phonon blocking and charge transmitting via the endotaxial placement of nanocrystals in a thermoelectric material host. Endotaxially arranged SrTe nanocrystals at concentrations as low as 2% were incorporated in a PbTe matrix doped with Na2Te. This effectively inhibits the heat flow in the system but does not affect the hole mobility, allowing a large power factor to be achieved. The crystallographic alignment of SrTe and PbTe lattices decouples phonon and electron transport and this allows the system to reach a thermoelectric figure of merit of 1.7 at ~800 K.

Access optionsAccess options

Rent or Buy article

Get time limited or full article access on ReadCube.

from$8.99

All prices are NET prices.

References

  1. 1.

    , , , & Recent development in thermoelectric materials. Int. Matter. Rev. 48, 45–66 (2003).

  2. 2.

    CRC Handbook of Thermoelectrics: Macro to Nano (CRC Press/Taylor & Francis, 2006).

  3. 3.

    & Complex thermoelctric materials. Nature Mater. 7, 105–114 (2008).

  4. 4.

    , & New and old concepts in thermoelectric materials. Angew. Chem. Int. Ed. 48, 8616–8639 (2009).

  5. 5.

    et al. Enhancement of thermoelectric efficiency in PbTe by distortion of the electronic density of states. Science 321, 554–557 (2008).

  6. 6.

    , & Ab Initio study of deep defect states in narrow band-gap semiconductors: group III impurities in PbTe. Phys. Rev. Lett. 96, 56403(1–4) (2006).

  7. 7.

    et al. Large enhancement in the power factor of bulk PbTe at high temperature by synergistic nanostructuring. Angew. Chem. Int. Ed. 47, 8618–8622 (2008).

  8. 8.

    et al. Cubic AgPbmSbTe2+m: bulk thermoelectric materials with high figure of merit. Science 303, 818–821 (2004).

  9. 9.

    et al. Nanostructuring, compositional fluctuations, and atomic ordering in the thermoelectric materials AgPbmSbTe2+m. The myth of solid solutions. J. Am. Chem. Soc. 127, 9177–9190 (2005).

  10. 10.

    , & Nanostructured AgPbmSbTe2+m system bulk materials with enhanced thermoelectric performance. J. Am. Chem. Soc. 130, 4527–4532 (2008).

  11. 11.

    et al. Nanostructuring and high thermoelectric efficiency in p-type Ag(Pb1-ySny)mSbTe2+m. Adv. Mater. 18, 1170–1173 (2006).

  12. 12.

    et al. High thermoelectric figure of merit and nanostructuring in bulk p-type Na1-xPbmSbyTe2+m. Angew. Chem. Int. Ed. 45, 3835–3839 (2006).

  13. 13.

    et al. Spinoidal decomposition and nucleation and growth as a means to bulk nanostructured thermoelectric: enhanced performance in Pb1-xSnxTePbS. J. Am. Chem. Soc. 129, 9780–9788 (2007).

  14. 14.

    et al. High-thermoelectric performance of nanostructured bismuth antimony telluride bulk alloys. Science 320, 634–638 (2008).

  15. 15.

    , , & Thin-film thermoelectric devices with high room-temperature figures of merit. Nature 413, 597–602 (2001).

  16. 16.

    New materials and performance limits for thermoelectric cooling. In CRC Hand Book of Thermoelectrics (Ed. D. M. Rowe), 407–440 (CRC Press, Boca Raton, 1995).

  17. 17.

    & Hall coefficient behavior and second valence band in lead telluride. J. Appl. Phys. 37, 302–309 (1966).

  18. 18.

    , & Semiconducting Lead Chalcogenides (Plenum, New York, vol. 5, 1970).

  19. 19.

    & Valence band structure of PbTe. J. Phys. Colloques 29, C4-129–C4-132 (1968).

  20. 20.

    , , , & Electrical transport properties of thallium-doped p-type PbTe films. Thin Solid Films 78, 153–159 (1981).

  21. 21.

    Temperature dependence of the energy gap in semiconductors. Physica 34, 149–154 (1967).

  22. 22.

    The Hall mobility and thermoelectric power of p-type lead telluride. Brit. J. Appl. Phys. 18, 1227–1235 (1967).

  23. 23.

    et al. Carrier concentration and temperature dependence of the electronic transport properties of epitaxial PbTe and PbTe/PbSe nanodot superlattice. Phys. Rev. B 77, 235202-1-14 (2008).

  24. 24.

    , & Lead strontium telluride and lead barium telluride grown by molecular-beam epitaxy. J. Vac. Sci. Technol. B 5, 686–689 (1987).

  25. 25.

    , & Quantitative measurement of displacement and strain fields from HREM micrographs. Ultramicroscopy 74, 131–146 (1998).

  26. 26.

    & Effect of point imperfections on lattice thermal conductivity. Phys. Rev. 120, 1149–1154 (1960).

  27. 27.

    & Estimation of the isotope effect on the lattice thermal conductivity of group IV and group III-V semiconductors. Phys. Rev. B 66, 195304 (2002).

  28. 28.

    , , & Thermal conductivity 27/thermal expansion 15 (Eds. Huang, H. & Porter, W.) 263–269 (DEStech Publication, 2004).

  29. 29.

    , , & Phonon engineering in nanostructures for solid-state energy conversion. Mat. Sci. Eng. A 292, 155–161 (2000).

  30. 30.

    & Phonon scattering cross section of polydispersed spherical nanoparticles. J. Appl. Phys. 99, 084306 (2006).

  31. 31.

    , , , & ‘Nanoparticle-in-Alloy’ approach to efficient thermoelectrics: silicides in SiGe. Nano Letters 9, 711–715 (2009).

  32. 32.

    , , & Microstructure-lattice thermal conductivity correlation in nanostructured PbTe0.7S0.3 thermoelectric material. Adv. Fun. Mater 20, 764–772 (2010).

  33. 33.

    Materials for thermoelectric energy conversion. Rep. Prog. Phys. 51, 459–539 (1988).

  34. 34.

    , , , & Disordered zinc in Zn4Sb3 with phonon-glass and electron-crystal thermoelectric properties. Nature Mater. 3, 458–463 (2004).

Download references

Acknowledgements

This work was supported by the Office of Naval Research (grant N00014-08-1-0613). Transmission electron microscopy work was performed in the (EPIC) (NIFTI) (Keck-II) facility of NUANCE Center at Northwestern University. NUANCE Center is supported by NSF-NSEC, NSF-MRSEC, Keck Foundation, the State of Illinois, and Northwestern University. The work at the University of Michigan is supported as part of the Revolutionary Materials for Solid State Energy Conversion, an Energy frontier Research Center funded by the U. S. Department of Energy, Office of Basic Energy Sciences under Award Number DE-SC0001054.

Author information

Affiliations

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

    • Kanishka Biswas
    • , Jiaqing He
    • , Qichun Zhang
    •  & Mercouri G. Kanatzidis
  2. Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA

    • Jiaqing He
    •  & Vinayak P. Dravid
  3. Department of Physics, University of Michigan, Ann Arbor, Michigan 48109, USA

    • Guoyu Wang
    •  & Ctirad Uher
  4. Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA

    • Mercouri G. Kanatzidis

Authors

  1. Search for Kanishka Biswas in:

  2. Search for Jiaqing He in:

  3. Search for Qichun Zhang in:

  4. Search for Guoyu Wang in:

  5. Search for Ctirad Uher in:

  6. Search for Vinayak P. Dravid in:

  7. Search for Mercouri G. Kanatzidis in:

Contributions

K.B., Q.Z. and M.G.K. prepared the samples, designed and carried out thermoelectric experiments. K.B. and M.G.K. analysed the electrical and thermal transport data. J.H. and V.P.D. carried out the TEM experiment and analysed the TEM data. G.W. and C.U. carried out the Hall measurements. K.B., J.H., V.P.D. and M.G.K. wrote the manuscript. All authors have reviewed, discussed and approved the results and conclusions of this article.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to Mercouri G. Kanatzidis.

Supplementary information

PDF files

  1. 1.

    Supplementary information

    Supplementary information

About this article

Publication history

Received

Accepted

Published

DOI

https://doi.org/10.1038/nchem.955