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A new class of doped nanobulk high-figure-of-merit thermoelectrics by scalable bottom-up assembly

Nature Materials volume 11, pages 233–240 (2012)Cite this article

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Abstract

Obtaining thermoelectric materials with high figure of merit ZT is an exacting challenge because it requires the independent control of electrical conductivity, thermal conductivity and Seebeck coefficient, which are often unfavourably coupled. Recent works have devised strategies based on nanostructuring and alloying to address this challenge in thin films, and to obtain bulk p-type alloys with ZT>1. Here, we demonstrate a new class of both p- and n-type bulk nanomaterials with room-temperature ZT as high as 1.1 using a combination of sub-atomic-per-cent doping and nanostructuring. Our nanomaterials were fabricated by bottom-up assembly of sulphur-doped pnictogen chalcogenide nanoplates sculpted by a scalable microwave-stimulated wet-chemical method. Bulk nanomaterials from single-component assemblies or nanoplate mixtures of different materials exhibit 25–250% higher ZT than their non-nanostructured bulk counterparts and state-of-the-art alloys. Adapting our synthesis and assembly approach should enable nanobulk thermoelectrics with further increases in ZT for transforming thermoelectric refrigeration and power harvesting technologies.

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Figure 1: Schematic representation of the scalable synthesis used to obtain both n- and p-type bulk thermoelectric nanomaterials with high figures of merit.
Figure 2: Figures of merit ZT for single-component and multicomponent bulk nanostructured pnictogen chalcogenides.
Figure 3: Single-crystal hexagonal pnictogen chalcogenide nanoplates and mercaptan-mediated sulphur injection.
Figure 4: Thermoelectric characterization of bulk-nanostructured pnictogen chalcogenides.
Figure 5: Diminution of lattice thermal conductivity in bulk-nanostructured chalcogenides due to nanoscale grain size and porosity.

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Acknowledgements

We gratefully acknowledge funding from the US Department of Energy, Office of Basic Energy Sciences through the S3TEC Energy Frontiers Research Center at MIT under Award DE-SC0001299, National Science Foundation grants DMR 0519081, ECCS 1002282 and CBET 0348613, and a gift grant from IBM through the Rensselaer Nanotechnology Center. We thank J. Woicik, B. Karlin and D. Fischer for help with setting up the photoemission experiments carried out at the National Synchrotron Light Source at Brookhaven National Laboratory, supported under the US Department of Energy contract DE-AC02-98CH10886. We thank J. Sharp at Marlow Industries and Z. Ren at Boston College for independently verifying our measured thermoelectric property values.

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Authors and Affiliations

  1. Materials Science and Engineering Department, Rensselaer Polytechnic Institute, 110 8th St., Troy, New York 12180, USA

    Rutvik J. Mehta, Chinnathambi Karthik, Binay Singh, Richard W. Siegel & Ganpati Ramanath

  2. Department of Mechanical, Aerospace and Nuclear Engineering, Rensselaer Polytechnic Institute, 110 8th St., Troy, New York 12180, USA

    Yanliang Zhang & Theodorian Borca-Tasciuc

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  1. Rutvik J. Mehta
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Contributions

R.J.M. carried out experiments, synthesized and characterized the materials and wrote the paper with G.R. Thermoelectric measurements and modelling were carried out by Y.Z. Data interpretation and analysis was carried out collaboratively by R.J.M., Y.Z., G.R. and T.B-T. C.K. and B.S. carried out transmission electron microscopy and X-ray photoelectron spectroscopy measurements, respectively. G.R. directed the project together with T.B-T. and R.W.S. All authors discussed the results and implications and commented on the manuscript at all stages.

Corresponding authors

Correspondence to Theodorian Borca-Tasciuc or Ganpati Ramanath.

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Mehta, R., Zhang, Y., Karthik, C. et al. A new class of doped nanobulk high-figure-of-merit thermoelectrics by scalable bottom-up assembly. Nature Mater 11, 233–240 (2012). https://doi.org/10.1038/nmat3213

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