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Title: Giant Pressure-Induced Enhancement of Seebeck Coefficient and Thermoelectric Efficiency in SnTe

Abstract

The thermoelectric properties of polycrystalline SnTe have been measured up to 4.5 GPa at 330 K. SnTe shows an enormous enhancement in Seebeck coefficient, greater than 200 % after 3 GPa, which correlates to a known pressure-induced structural phase transition that is observed through simultaneous in situ X-ray diffraction measurement. We also measured electrical resistance and relative changes to the thermal conductivity, enabling the determination of relative changes in the dimensionless figure of merit (ZT), which increases dramatically after 3 GPa, reaching 350 % of the lowest pressure ZT value. Our results demonstrate a fundamental relationship between structure and thermoelectric behaviours and suggest that pressure is an effective tool to control them.

Authors:
 [1];  [1]; ORCiD logo [2];  [2];  [1]; ORCiD logo [3]
  1. Univ. of Nevada, Las Vegas, NV (United States). High Pressure Science and Engineering Center (HiPSEC), Dept. of Physics and Astronomy
  2. Carnegie Inst. of Washington, Argonne, IL (United States). Geophysical Lab.
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1408846
Report Number(s):
LA-UR-17-28893
Journal ID: ISSN 1439-4235; TRN: US1702956
Grant/Contract Number:
AC52-06NA25396; NA0001982; NA0001974; AC02-06CH11357; FG02-99ER45775
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ChemPhysChem
Additional Journal Information:
Journal Volume: 18; Journal Issue: 23; Journal ID: ISSN 1439-4235
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; materials science; pressure; Seebeck coefficient; SnTe; thermoelectric efficiency

Citation Formats

Baker, Jason, Kumar, Ravhi, Park, Changyong, Kenney-Benson, Curtis, Cornelius, Andrew, and Velisavljevic, Nenad. Giant Pressure-Induced Enhancement of Seebeck Coefficient and Thermoelectric Efficiency in SnTe. United States: N. p., 2017. Web. doi:10.1002/cphc.201700994.
Baker, Jason, Kumar, Ravhi, Park, Changyong, Kenney-Benson, Curtis, Cornelius, Andrew, & Velisavljevic, Nenad. Giant Pressure-Induced Enhancement of Seebeck Coefficient and Thermoelectric Efficiency in SnTe. United States. doi:10.1002/cphc.201700994.
Baker, Jason, Kumar, Ravhi, Park, Changyong, Kenney-Benson, Curtis, Cornelius, Andrew, and Velisavljevic, Nenad. 2017. "Giant Pressure-Induced Enhancement of Seebeck Coefficient and Thermoelectric Efficiency in SnTe". United States. doi:10.1002/cphc.201700994.
@article{osti_1408846,
title = {Giant Pressure-Induced Enhancement of Seebeck Coefficient and Thermoelectric Efficiency in SnTe},
author = {Baker, Jason and Kumar, Ravhi and Park, Changyong and Kenney-Benson, Curtis and Cornelius, Andrew and Velisavljevic, Nenad},
abstractNote = {The thermoelectric properties of polycrystalline SnTe have been measured up to 4.5 GPa at 330 K. SnTe shows an enormous enhancement in Seebeck coefficient, greater than 200 % after 3 GPa, which correlates to a known pressure-induced structural phase transition that is observed through simultaneous in situ X-ray diffraction measurement. We also measured electrical resistance and relative changes to the thermal conductivity, enabling the determination of relative changes in the dimensionless figure of merit (ZT), which increases dramatically after 3 GPa, reaching 350 % of the lowest pressure ZT value. Our results demonstrate a fundamental relationship between structure and thermoelectric behaviours and suggest that pressure is an effective tool to control them.},
doi = {10.1002/cphc.201700994},
journal = {ChemPhysChem},
number = 23,
volume = 18,
place = {United States},
year = 2017,
month =
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on October 30, 2018
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  • The thermoelectric properties of polycrystalline SnTe have been measured up to 4.5 GPa at 330 K. SnTe shows an enormous enhancement in Seebeck coefficient, greater than 200 % after 3 GPa, which correlates to a known pressure-induced structural phase transition that is observed through simultaneous in situ X-ray diffraction measurement. Electrical resistance and relative changes to the thermal conductivity were also measured, enabling the determination of relative changes in the dimensionless figure of merit (ZT), which increases dramatically after 3 GPa, reaching 350 % of the lowest pressure ZT value. The results demonstrate a fundamental relationship between structure and thermoelectricmore » behaviours and suggest that pressure is an effective tool to control them.« less
  • The thermo-emf {delta}V and current {delta}I generated by imposing the alternating temperature gradients (ATG) at a period of T and the steady temperature gradient (STG) on a thermoelectric (TE) composite were measured as a function of t, where t is the lapsed time and T was varied from 60 to or {infinity} s. The STG and ATG were produced by imposing steadily and alternatively a source voltage V in the range from 1.0 to 4.0 V on two Peltier modules sandwiching a composite. {delta}T, {delta}V, {delta}I and V{sub P} oscillate at a period T and their waveforms vary significantly withmore » a change of T, where {delta}V and V{sub P} are the voltage drops in a load resistance R{sub L} and in resistance R{sub P} of two modules. The resultant Seebeck coefficient |{alpha}| = |{delta}V|/{delta}T of a composite under the STG was found to be expressed as |{alpha}| = |{alpha}{sub 0}|(1 - R{sub comp}/R{sub T}), where R{sub T} is the total resistance of a circuit for measuring the output signals and R{sub comp} is the resistance of a composite. The effective generating power {delta}W{sub eff} has a local maximum at T = 960 s for the p-type composite and at T = 480 s for the n-type one. The maximum energy conversion efficiency {eta} of the p- and n-type composites under the ATG produced by imposing a voltage of 4.0 V at an optimum period were 0.22 and 0.23% at {delta}T{sub eff} = 50 K, respectively, which are 42 and 43% higher than those at {delta}T = 42 K under the STG. These maximum {eta} for a TE composite sandwiched between two Peltier modules, were found to be expressed theoretically in terms of R{sub P}, R{sub T}, R{sub L}, {alpha}{sub P} and {alpha}, where {alpha}{sub P} and {alpha} are the resultant Seebeck coefficients of Peltier modules and a TE composite.« less
  • We report a significant enhancement of the thermoelectric performance of p-type SnTe over a broad temperature plateau with a peak ZT value of similar to 1.4 at 923 K through In/Cd codoping and a CdS nanostructuring approach. Indium and cadmium play different but complementary roles in modifying the valence band structure of SnTe. Specifically, In-doping introduces resonant levels inside the valence bands, leading to a considerably improved Seebeck coefficient at low temperature. Cd-doping, however, increases the Seebeck coefficient of SnTe remarkably in the mid- to high-temperature region via a convergence of the light and heavy hole bands and an enlargementmore » of the band gap. Combining the two dopants in SnTe yields enhanced Seebeck coefficient and power factor over a wide temperature range due to the synergy of resonance levels and valence band convergence, as demonstrated by the Pisarenko plot and supported by first-principles band structure calculations. Moreover, these codoped samples can be hierarchically structured on all scales (atomic point defects by doping, nanoscale precipitations by CdS nanostructuring, and mesoscale grains by SPS treatment) to achieve highly effective phonon scattering leading to strongly reduced thermal conductivities. In addition to the high maximum ZT the resultant large average ZT of similar to 0.8 between 300 and 923 K makes SnTe an attractive p-type material for high-temperature thermoelectric power generation.« less