TY - JOUR
T1 - High-performance bulk thermoelectrics with all-scale hierarchical architectures
AU - Biswas, Kanishka
AU - He, Jiaqing
AU - Blum, Ivan D.
AU - Wu, Chun I.
AU - Hogan, Timothy P.
AU - Seidman, David N.
AU - Dravid, Vinayak P.
AU - Kanatzidis, Mercouri G.
N1 - Funding Information:
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.
PY - 2012/9/20
Y1 - 2012/9/20
N2 - 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 1.51.8 at 750900 kelvin, 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 fashionfrom atomic-scale lattice disorder and nanoscale endotaxial precipitates to mesoscale grain boundarieswe 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.
AB - 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 1.51.8 at 750900 kelvin, 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 fashionfrom atomic-scale lattice disorder and nanoscale endotaxial precipitates to mesoscale grain boundarieswe 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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U2 - 10.1038/nature11439
DO - 10.1038/nature11439
M3 - Article
C2 - 22996556
AN - SCOPUS:84866505161
VL - 489
SP - 414
EP - 418
JO - Nature
JF - Nature
SN - 0028-0836
IS - 7416
ER -