Thermoelectrics from abundant chemical elements: High-performance nanostructured PbSe-PbS

John Androulakis, Iliya Todorov, Jiaqing He, Duck Young Chung, Vinayak P Dravid, Mercouri Kanatzidis*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

130 Scopus citations

Abstract

We report promising thermoelectric properties of the rock salt PbSe-PbS system which consists of chemical elements with high natural abundance. Doping with PbCl2, excess Pb, and Bi gives n-type behavior without significantly perturbing the cation sublattice. Thus, despite the great extent of dissolution of PbS in PbSe, the transport properties in this system, such as carrier mobilities and power factors, are remarkably similar to those of pristine n-type PbSe in fractions as high as 16%. The unexpected finding is the presence of precipitates ∼2-5 nm in size, revealed by transmission electron microscopy, that increase in density with increasing PbS concentration, in contrast to previous reports of the occurrence of a complete solid solution in this system. We report a marked impact of the observed nanostructuring on the lattice thermal conductivity, as highlighted by contrasting the experimental values (∼1.3 W/mK) to those predicted by Klemens-Drabble theory at room temperature (∼1.6 W/mK). Our thermal conductivity results show that, unlike in PbTe, optical phonon excitations in PbSe-PbS systems contribute to heat transport at all temperatures. We show that figures of merit reaching as high as ∼1.2-1.3 at 900 K can be obtained, suggesting that large-scale applications with good conversion efficiencies are possible from systems based on abundant, inexpensive chemical elements.

Original languageEnglish (US)
Pages (from-to)10920-10927
Number of pages8
JournalJournal of the American Chemical Society
Volume133
Issue number28
DOIs
StatePublished - Jul 20 2011

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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