Superior thermoelectric performance in PbTe-PbS pseudo-binary

Extremely low thermal conductivity and modulated carrier concentration

Di Wu, Li Dong Zhao, Xiao Tong, Wei Li, Lijun Wu, Qing Tan, Yanling Pei, Li Huang, Jing Feng Li, Yimei Zhu, Mercouri G. Kanatzidis, Jiaqing He

Research output: Contribution to journalArticle

76 Citations (Scopus)

Abstract

Lead chalcogenides are dominant thermoelectric materials in the medium-temperature range due to their highly favorable electronic band structures and low thermal conductivities. An important system is the PbTe-PbS pseudo-binary, and its low thermal conductivity originates largely from the coexistence of both alloying and nanostructuring through phase-separation. To better understand the competition between the alloying and phase separation and its pronounced effects on the thermoelectric performance in PbTe-PbS, we systematically studied, via transmission electron microscopy (TEM) observations and theoretical calculations, the samples of Spark Plasma Sintered (SPSed) 3 at% Na-doped (PbTe)1-x(PbS)x with x = 10%, 15%, 20%, 25%, 30% and 35%. The highest figure of merit, viz., ZT ∼ 2.3 was obtained at 923 K, when the PbS phase-fraction, x, was 20%, which corresponds to the lowest lattice thermal conductivity of the series. The consistently lower lattice thermal conductivities in the SPSed samples as compared with the corresponding ingots originates from the mesostructured nature of the former, which contributes significantly to their superior ZT. We also studied the onset of carrier concentration modulation at ∼600 K, which leads to the observed saturation of electrical transport properties due to the diffusion and re-dissolution of excessive Na into the PbTe-PbS matrix. This carrier concentration modulation is equally crucial to achieve very high power factors (up to 26.5 μW cm-1 K-2 at 623 K) and outstanding thermoelectric performances in SPSed PbTe-PbS binaries.

Original languageEnglish
Pages (from-to)2056-2068
Number of pages13
JournalEnergy and Environmental Science
Volume8
Issue number7
DOIs
Publication statusPublished - Jul 1 2015

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thermal conductivity
Carrier concentration
Thermal conductivity
Electric sparks
Plasmas
Alloying
plasma
Phase separation
Modulation
Chalcogenides
Ingots
Band structure
Transport properties
coexistence
transmission electron microscopy
Dissolution
Lead
dissolution
saturation
Transmission electron microscopy

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Environmental Chemistry
  • Pollution
  • Nuclear Energy and Engineering

Cite this

Superior thermoelectric performance in PbTe-PbS pseudo-binary : Extremely low thermal conductivity and modulated carrier concentration. / Wu, Di; Zhao, Li Dong; Tong, Xiao; Li, Wei; Wu, Lijun; Tan, Qing; Pei, Yanling; Huang, Li; Li, Jing Feng; Zhu, Yimei; Kanatzidis, Mercouri G.; He, Jiaqing.

In: Energy and Environmental Science, Vol. 8, No. 7, 01.07.2015, p. 2056-2068.

Research output: Contribution to journalArticle

Wu, Di ; Zhao, Li Dong ; Tong, Xiao ; Li, Wei ; Wu, Lijun ; Tan, Qing ; Pei, Yanling ; Huang, Li ; Li, Jing Feng ; Zhu, Yimei ; Kanatzidis, Mercouri G. ; He, Jiaqing. / Superior thermoelectric performance in PbTe-PbS pseudo-binary : Extremely low thermal conductivity and modulated carrier concentration. In: Energy and Environmental Science. 2015 ; Vol. 8, No. 7. pp. 2056-2068.
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