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

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

doi:10.1002/aenm.201803242

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

Journal Article · Tue Jan 29 00:00:00 EST 2019 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201803242· OSTI ID:1530602

Shi, Xiaolei -L. ^[1]; Wu, Angyin -Y. ^[1]; Feng, Tianli ^[2]; Zheng, Kun ^[3]; Liu, Weidi -D. ^[1]; Sun, Qiang ^[1]; Hong, Min ^[4]; Pantelides, Sokrates T. ^[2];

^[5]; Zou, Jin ^[6]

Univ. of Queensland, Brisbane, QLD (Australia). Materials Engineering
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
Beijing Univ. of Technology (China). Inst. of Microstructure and Properties of Advanced Materials, Beijing Key Lab. of Microstructure and Property of Solids
Univ. of Southern Queensland, Springfield Central, QLD (Australia). Centre for Future Materials
Univ. of Queensland, Brisbane, QLD (Australia). Materials Engineering; Univ. of Southern Queensland, Springfield Central, QLD (Australia). Centre for Future Materials
Univ. of Queensland, Brisbane, QLD (Australia). Materials Engineering, and Centre for Microscopy and Microanalysis

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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Vanderbilt Univ., Nashville, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: FG0209ER46554; AC02-05CH11231; FG02-09ER46554

OSTI ID:: 1530602

Alternate ID(s):: OSTI ID: 1492745; OSTI ID: 1597926

Journal Information:: Advanced Energy Materials, Vol. 9, Issue 11; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 153 works

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