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Title: High Thermoelectric Performance in p-type Polycrystalline Cd-doped SnSe Achieved by a Combination of Cation Vacancies and Localized Lattice Engineering

Abstract

In this paper, a high figure of merit (ZT) of ≈1.7 at 823 K is reported in p-type polycrystalline Cd-doped SnSe by combining cation vacancies and localized-lattice engineering. It is observed that the introduction of Cd atoms in SnSe lattice induce Sn vacancies, which act as p-type dopants. A combination of facile solvothermal synthesis and fast spark plasma sintering technique boosts the Sn vacancy to a high level of ≈2.9%, which results in an optimum hole concentration of ≈2.6 × 1019 cm-3 and an improved power factor of ≈6.9 µW cm-1 K-2. Simultaneously, a low thermal conductivity of ≈0.33 W m-1 K-1 is achieved by effective phonon scattering at localized crystal imperfections, as observed by detailed structural characterizations. Density functional theory calculations reveal that the role of Cd atoms in the SnSe lattice is to reduce the formation energy of Sn vacancies, which in turn lower the Fermi level down into the valence bands, generating holes. This work explores the fundamental Cd-doping mechanisms at the nanoscale in a SnSe matrix and demonstrates vacancy and localized-lattice engineering as an effective approach to boosting thermoelectric performance. The work provides an avenue in achieving high-performance thermoelectric properties of materials.

Authors:
 [1];  [1];  [2];  [3];  [1];  [1];  [4];  [2]; ORCiD logo [5];  [6]
  1. Univ. of Queensland, Brisbane, QLD (Australia). Materials Engineering
  2. Vanderbilt Univ., Nashville, TN (United States). Dept. of Physics and Astronomy, and Dept. of Electrical Engineering and Computer Science; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  3. Beijing Univ. of Technology (China). Inst. of Microstructure and Properties of Advanced Materials, Beijing Key Lab. of Microstructure and Property of Solids
  4. Univ. of Southern Queensland, Springfield Central, QLD (Australia). Centre for Future Materials
  5. Univ. of Queensland, Brisbane, QLD (Australia). Materials Engineering; Univ. of Southern Queensland, Springfield Central, QLD (Australia). Centre for Future Materials
  6. Univ. of Queensland, Brisbane, QLD (Australia). Materials Engineering, and Centre for Microscopy and Microanalysis
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Vanderbilt Univ., Nashville, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1530602
Alternate Identifier(s):
OSTI ID: 1492745; OSTI ID: 1597926
Grant/Contract Number:  
FG0209ER46554; AC02-05CH11231; FG02-09ER46554
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 11; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Cd-doping; characterization; solvothermal; thermoelectric; tin selenide

Citation Formats

Shi, Xiaolei -L., Wu, Angyin -Y., Feng, Tianli, Zheng, Kun, Liu, Weidi -D., Sun, Qiang, Hong, Min, Pantelides, Sokrates T., Chen, Zhi-Gang, and Zou, Jin. High Thermoelectric Performance in p-type Polycrystalline Cd-doped SnSe Achieved by a Combination of Cation Vacancies and Localized Lattice Engineering. United States: N. p., 2019. Web. doi:10.1002/aenm.201803242.
Shi, Xiaolei -L., Wu, Angyin -Y., Feng, Tianli, Zheng, Kun, Liu, Weidi -D., Sun, Qiang, Hong, Min, Pantelides, Sokrates T., Chen, Zhi-Gang, & Zou, Jin. High Thermoelectric Performance in p-type Polycrystalline Cd-doped SnSe Achieved by a Combination of Cation Vacancies and Localized Lattice Engineering. United States. https://doi.org/10.1002/aenm.201803242
Shi, Xiaolei -L., Wu, Angyin -Y., Feng, Tianli, Zheng, Kun, Liu, Weidi -D., Sun, Qiang, Hong, Min, Pantelides, Sokrates T., Chen, Zhi-Gang, and Zou, Jin. Tue . "High Thermoelectric Performance in p-type Polycrystalline Cd-doped SnSe Achieved by a Combination of Cation Vacancies and Localized Lattice Engineering". United States. https://doi.org/10.1002/aenm.201803242. https://www.osti.gov/servlets/purl/1530602.
@article{osti_1530602,
title = {High Thermoelectric Performance in p-type Polycrystalline Cd-doped SnSe Achieved by a Combination of Cation Vacancies and Localized Lattice Engineering},
author = {Shi, Xiaolei -L. and Wu, Angyin -Y. and Feng, Tianli and Zheng, Kun and Liu, Weidi -D. and Sun, Qiang and Hong, Min and Pantelides, Sokrates T. and Chen, Zhi-Gang and Zou, Jin},
abstractNote = {In this paper, a high figure of merit (ZT) of ≈1.7 at 823 K is reported in p-type polycrystalline Cd-doped SnSe by combining cation vacancies and localized-lattice engineering. It is observed that the introduction of Cd atoms in SnSe lattice induce Sn vacancies, which act as p-type dopants. A combination of facile solvothermal synthesis and fast spark plasma sintering technique boosts the Sn vacancy to a high level of ≈2.9%, which results in an optimum hole concentration of ≈2.6 × 1019 cm-3 and an improved power factor of ≈6.9 µW cm-1 K-2. Simultaneously, a low thermal conductivity of ≈0.33 W m-1 K-1 is achieved by effective phonon scattering at localized crystal imperfections, as observed by detailed structural characterizations. Density functional theory calculations reveal that the role of Cd atoms in the SnSe lattice is to reduce the formation energy of Sn vacancies, which in turn lower the Fermi level down into the valence bands, generating holes. This work explores the fundamental Cd-doping mechanisms at the nanoscale in a SnSe matrix and demonstrates vacancy and localized-lattice engineering as an effective approach to boosting thermoelectric performance. The work provides an avenue in achieving high-performance thermoelectric properties of materials.},
doi = {10.1002/aenm.201803242},
journal = {Advanced Energy Materials},
number = 11,
volume = 9,
place = {United States},
year = {Tue Jan 29 00:00:00 EST 2019},
month = {Tue Jan 29 00:00:00 EST 2019}
}

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