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Title: High Thermoelectric Performance in SnTe–AgSbTe2 Alloys from Lattice Softening, Giant Phonon–Vacancy Scattering, and Valence Band Convergence

Abstract

We report on the underlying mechanism that enables the SnTe-AgSbTe2 system to exhibit superior thermoelectric figure of merit (ZT) compared to its parent compound SnTe. We show that AgSbTe2 alloying has a profound impact on the band structure of SnTe by converging the energies of its light and heavy valence bands, leading to significantly enhanced Seebeck coefficients. We have also unraveled a significant connection between alloying and defect stability in this system, wherein the Sn vacancy concentration increases significantly when Ag and Sb are alloyed on the Sn site. The increased Sn vacancy concentration dramatically reduces the lattice thermal conductivity through both lattice softening and phonon-vacancy scattering to ~0.4 W m-1 K-1 at 800 K. Consequently, a ZT value of 1.2 at 800 K for AgSn5SbTe7 can be achieved by doping I on Te sites. Lastly, this represents a 300% improvement over pristine SnTe, outperforming many reported SnTe-based thermoelectric materials.

Authors:
ORCiD logo [1];  [2];  [2];  [2];  [2];  [3]; ORCiD logo [4]; ORCiD logo [5];  [3]; ORCiD logo [2];  [2]; ORCiD logo [2]; ORCiD logo [6]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  2. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
  3. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Physics
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  5. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Wuhan Univ. of Technology (China). State Key Lab. of Advanced Technology for Materials Synthesis and Processing
  6. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1459892
Grant/Contract Number:  
AC02-06CH11357; SC0014520
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 3; Journal Issue: 3; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Tan, Gangjian, Hao, Shiqiang, Hanus, Riley C., Zhang, Xiaomi, Anand, Shashwat, Bailey, Trevor P., Rettie, Alexander J. E., Su, Xianli, Uher, Ctirad, Dravid, Vinayak P., Snyder, G. Jeffrey, Wolverton, Chris, and Kanatzidis, Mercouri G. High Thermoelectric Performance in SnTe–AgSbTe2 Alloys from Lattice Softening, Giant Phonon–Vacancy Scattering, and Valence Band Convergence. United States: N. p., 2018. Web. doi:10.1021/acsenergylett.8b00137.
Tan, Gangjian, Hao, Shiqiang, Hanus, Riley C., Zhang, Xiaomi, Anand, Shashwat, Bailey, Trevor P., Rettie, Alexander J. E., Su, Xianli, Uher, Ctirad, Dravid, Vinayak P., Snyder, G. Jeffrey, Wolverton, Chris, & Kanatzidis, Mercouri G. High Thermoelectric Performance in SnTe–AgSbTe2 Alloys from Lattice Softening, Giant Phonon–Vacancy Scattering, and Valence Band Convergence. United States. doi:10.1021/acsenergylett.8b00137.
Tan, Gangjian, Hao, Shiqiang, Hanus, Riley C., Zhang, Xiaomi, Anand, Shashwat, Bailey, Trevor P., Rettie, Alexander J. E., Su, Xianli, Uher, Ctirad, Dravid, Vinayak P., Snyder, G. Jeffrey, Wolverton, Chris, and Kanatzidis, Mercouri G. Mon . "High Thermoelectric Performance in SnTe–AgSbTe2 Alloys from Lattice Softening, Giant Phonon–Vacancy Scattering, and Valence Band Convergence". United States. doi:10.1021/acsenergylett.8b00137. https://www.osti.gov/servlets/purl/1459892.
@article{osti_1459892,
title = {High Thermoelectric Performance in SnTe–AgSbTe2 Alloys from Lattice Softening, Giant Phonon–Vacancy Scattering, and Valence Band Convergence},
author = {Tan, Gangjian and Hao, Shiqiang and Hanus, Riley C. and Zhang, Xiaomi and Anand, Shashwat and Bailey, Trevor P. and Rettie, Alexander J. E. and Su, Xianli and Uher, Ctirad and Dravid, Vinayak P. and Snyder, G. Jeffrey and Wolverton, Chris and Kanatzidis, Mercouri G.},
abstractNote = {We report on the underlying mechanism that enables the SnTe-AgSbTe2 system to exhibit superior thermoelectric figure of merit (ZT) compared to its parent compound SnTe. We show that AgSbTe2 alloying has a profound impact on the band structure of SnTe by converging the energies of its light and heavy valence bands, leading to significantly enhanced Seebeck coefficients. We have also unraveled a significant connection between alloying and defect stability in this system, wherein the Sn vacancy concentration increases significantly when Ag and Sb are alloyed on the Sn site. The increased Sn vacancy concentration dramatically reduces the lattice thermal conductivity through both lattice softening and phonon-vacancy scattering to ~0.4 W m-1 K-1 at 800 K. Consequently, a ZT value of 1.2 at 800 K for AgSn5SbTe7 can be achieved by doping I on Te sites. Lastly, this represents a 300% improvement over pristine SnTe, outperforming many reported SnTe-based thermoelectric materials.},
doi = {10.1021/acsenergylett.8b00137},
journal = {ACS Energy Letters},
number = 3,
volume = 3,
place = {United States},
year = {2018},
month = {2}
}

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Cited by: 11 works
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Figures / Tables:

Table 1 Table 1: Room temperature physical properties, including mass density ($ρ$), Hall carrier concentrations ($N$$p$) and carrier mobilities ($μ$) for AgSnmSbTe2+m.

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.