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High-performance bulk thermoelectrics with all-scale hierarchical architectures

Nature volume 489, pages 414–418 (2012)Cite this article

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A Corrigendum to this article was published on 24 October 2012

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Abstract

With about two-thirds of all used energy being lost as waste heat, there is a compelling need for high-performance thermoelectric materials that can directly and reversibly convert heat to electrical energy. However, the practical realization of thermoelectric materials is limited by their hitherto low figure of merit, ZT, which governs the Carnot efficiency according to the second law of thermodynamics. The recent successful strategy of nanostructuring to reduce thermal conductivity has achieved record-high ZT values in the range 1.5–1.8 at 750–900 kelvin1,2,3, but still falls short of the generally desired threshold value of 2. Nanostructures in bulk thermoelectrics allow effective phonon scattering of a significant portion of the phonon spectrum, but phonons with long mean free paths remain largely unaffected. Here we show that heat-carrying phonons with long mean free paths can be scattered by controlling and fine-tuning the mesoscale architecture of nanostructured thermoelectric materials. Thus, by considering sources of scattering on all relevant length scales in a hierarchical fashion—from atomic-scale lattice disorder and nanoscale endotaxial precipitates to mesoscale grain boundaries—we achieve the maximum reduction in lattice thermal conductivity and a large enhancement in the thermoelectric performance of PbTe. By taking such a panoscopic approach to the scattering of heat-carrying phonons across integrated length scales, we go beyond nanostructuring and demonstrate a ZT value of ∼2.2 at 915 kelvin in p-type PbTe endotaxially nanostructured with SrTe at a concentration of 4 mole per cent and mesostructured with powder processing and spark plasma sintering. This increase in ZT beyond the threshold of 2 highlights the role of, and need for, multiscale hierarchical architecture in controlling phonon scattering in bulk thermoelectrics, and offers a realistic prospect of the recovery of a significant portion of waste heat.

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Figure 1: All-length-scale hierarchy in thermoelectric materials.
Figure 2: Thermoelectric properties of SPS and ingot samples of PbTe–SrTe doped with 2 mol% Na.
Figure 3: Micro and nanostructures in SPS PbTe–SrTe(4 mol%) doped with 2 mol% Na.
Figure 4: Compositional analysis of SPS PbTe–SrTe(4 mol%) doped with 2 mol% Na.

Change history

  • 24 October 2012

    Nature 489, 414–418 (2012); doi:10.1038/nature11439 In this Letter, the units of thermal conductivity on the y-axes of Fig. 2d and e should be W m−1 K−1 and the y-axis label of Fig. 3d should be ‘Count (%)’. Figures 2 and 3 of the original paper have been corrected online.

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Acknowledgements

This work was supported by the Energy Frontier Research Center for Revolutionary Materials for Solid State Energy Conversion, funded by the US Department of Energy, Office of Science, Basic Energy Sciences under award number DE-SC0001054. TEM was performed in the (EPIC) (NIFTI) (Keck-II) facility of the NUANCE Center at Northwestern University. The spark plasma sintering system at Michigan State University is supported by ONR DURIP. APT was performed at NUCAPT and supported by NSF-MRI (DMR-0420532), ONR-DURIP (N00014-0400798, N00014-0610539, N00014-0910781), MRSEC (DMR-1121262) and ISEN at Northwestern University.

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Author notes

  1. Kanishka Biswas & Jiaqing He

    Present address: Present addresses: New Chemistry Unit, Jawarharlal Nehru Centre for Advanced Scientific Research (JNCASR), Jakkur, Bangalore 560064, India (K.B.); Frantier Institute of Science and Technology (FIST), Xi'an Jiaotong University, Xi'an 710054, China (J.H.).,

Authors and Affiliations

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

    Kanishka Biswas, Jiaqing He & Mercouri G. Kanatzidis

  2. Materials Science and Engineering, Northwestern University, Evanston, 60208, Illinois, USA

    Jiaqing He, Ivan D. Blum, David N. Seidman & Vinayak P. Dravid

  3. Department of Electrical and Computer Engineering, Michigan State University, East Lansing, 48824, Michigan, USA

    Chun-I Wu & Timothy P. Hogan

  4. Materials Science Division, Argonne National Laboratory, Argonne, 60439, Illinois, USA

    Mercouri G. Kanatzidis

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Contributions

K.B. synthesized the samples and designed and carried out thermoelectric experiments. J.H. performed the TEM experiments. I.D.B. performed the APT measurements. C.-I.W. and T.P.H. performed the spark plasma sintering. K.B., J.H., I.D.B., D.N.S., V.P.D. and M.G.K. conceived the experiments, analysed the results and wrote and edited the manuscript.

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Correspondence to Mercouri G. Kanatzidis.

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Biswas, K., He, J., Blum, I. et al. High-performance bulk thermoelectrics with all-scale hierarchical architectures. Nature 489, 414–418 (2012). https://doi.org/10.1038/nature11439

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