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

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.

doi:10.1021/acsenergylett.8b00137

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

Journal Article · Mon Feb 12 00:00:00 EST 2018 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.8b00137· OSTI ID:1459892

^[1]; Hao, Shiqiang ^[2]; Hanus, Riley C. ^[2]; Zhang, Xiaomi ^[2]; Anand, Shashwat ^[2]; Bailey, Trevor P. ^[3];

^[4];

^[5]; Uher, Ctirad ^[3];

^[2]; Snyder, G. Jeffrey ^[2];

^[2];

^[6]

Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Physics
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
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
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division

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. This represents a 300% improvement over pristine SnTe, outperforming many reported SnTe-based thermoelectric materials.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0014520

OSTI ID:: 1459892

Alternate ID(s):: OSTI ID: 1775442

Journal Information:: ACS Energy Letters, Vol. 3, Issue 3; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 115 works

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

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