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Title: Subtle Roles of Sb and S in Regulating the Thermoelectric Properties of N-Type PbTe to High Performance

Abstract

A high ZT (thermoelectric figure of merit) of ≈1.4 at 900 K for n‐type PbTe is reported, through modifying its electrical and thermal properties by incorporating Sb and S, respectively. Sb is confirmed to be an amphoteric dopant in PbTe, filling Te vacancies at low doping levels (<1%), exceeding which it enters into Pb sites. It is found that Sb‐doped PbTe exhibits much higher carrier mobility than similar Bi‐doped materials, and accordingly, delivers higher power factors and superior ZT . The enhanced electronic transport is attributed to the elimination of Te vacancies, which appear to strongly scatter n‐type charge carriers. Building on this result, the ZT of Pb 0.9875 Sb 0.0125 Te is further enhanced by alloying S into the Te sublattice. The introduction of S opens the bandgap of PbTe, which suppresses bipolar conduction while simultaneously increasing the electron concentration and electrical conductivity. Furthermore, it introduces point defects and induces second phase nanostructuring, which lowers the lattice thermal conductivity to ≈0.5 W m −1 K −1 at 900 K, making this material a robust candidate for high‐temperature (500–900 K) thermoelectric applications. It is anticipated that the insights provided here will be an important addition to the growing arsenal ofmore » strategies for optimizing the performance of thermoelectric materials.« less

Authors:
ORCiD logo [1];  [1];  [2];  [3];  [4];  [3];  [1]
+ Show Author Affiliations
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  2. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Physics; Wuhan Univ. of Technology (China). State Key Lab. of Advanced Technology for Materials Synthesis and Processing
  3. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Physics
  4. Beihang Univ., Beijing (China). School of Materials Science and Engineering
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1395373
Alternate Identifier(s):
OSTI ID: 1393302
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 7; Journal Issue: 18; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
ENGLISH
Subject:
36 MATERIALS SCIENCE; thermoelectrics; thermal conductivity; n-type PbTe; doping

Citation Formats

Tan, Gangjian, Stoumpos, Constantinos C., Wang, Si, Bailey, Trevor P., Zhao, Li‐Dong, Uher, Ctirad, and Kanatzidis, Mercouri G. Subtle Roles of Sb and S in Regulating the Thermoelectric Properties of N-Type PbTe to High Performance. United States: N. p., 2017. Web. doi:10.1002/aenm.201700099.
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Tan, Gangjian, Stoumpos, Constantinos C., Wang, Si, Bailey, Trevor P., Zhao, Li‐Dong, Uher, Ctirad, & Kanatzidis, Mercouri G. Subtle Roles of Sb and S in Regulating the Thermoelectric Properties of N-Type PbTe to High Performance. United States. https://doi.org/10.1002/aenm.201700099
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Tan, Gangjian, Stoumpos, Constantinos C., Wang, Si, Bailey, Trevor P., Zhao, Li‐Dong, Uher, Ctirad, and Kanatzidis, Mercouri G. Mon . "Subtle Roles of Sb and S in Regulating the Thermoelectric Properties of N-Type PbTe to High Performance". United States. https://doi.org/10.1002/aenm.201700099. https://www.osti.gov/servlets/purl/1395373.
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@article{osti_1395373,
title = {Subtle Roles of Sb and S in Regulating the Thermoelectric Properties of N-Type PbTe to High Performance},
author = {Tan, Gangjian and Stoumpos, Constantinos C. and Wang, Si and Bailey, Trevor P. and Zhao, Li‐Dong and Uher, Ctirad and Kanatzidis, Mercouri G.},
abstractNote = {A high ZT (thermoelectric figure of merit) of ≈1.4 at 900 K for n‐type PbTe is reported, through modifying its electrical and thermal properties by incorporating Sb and S, respectively. Sb is confirmed to be an amphoteric dopant in PbTe, filling Te vacancies at low doping levels (<1%), exceeding which it enters into Pb sites. It is found that Sb‐doped PbTe exhibits much higher carrier mobility than similar Bi‐doped materials, and accordingly, delivers higher power factors and superior ZT . The enhanced electronic transport is attributed to the elimination of Te vacancies, which appear to strongly scatter n‐type charge carriers. Building on this result, the ZT of Pb 0.9875 Sb 0.0125 Te is further enhanced by alloying S into the Te sublattice. The introduction of S opens the bandgap of PbTe, which suppresses bipolar conduction while simultaneously increasing the electron concentration and electrical conductivity. Furthermore, it introduces point defects and induces second phase nanostructuring, which lowers the lattice thermal conductivity to ≈0.5 W m −1 K −1 at 900 K, making this material a robust candidate for high‐temperature (500–900 K) thermoelectric applications. It is anticipated that the insights provided here will be an important addition to the growing arsenal of strategies for optimizing the performance of thermoelectric materials.},
doi = {10.1002/aenm.201700099},
journal = {Advanced Energy Materials},
number = 18,
volume = 7,
place = {United States},
year = {Mon May 22 00:00:00 EDT 2017},
month = {Mon May 22 00:00:00 EDT 2017}
}
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