High Seebeck Coefficient and Unusually Low Thermal Conductivity Near Ambient Temperatures in Layered Compound Yb 2– x Eu x CdSb 2
Abstract
Zintl phases are promising thermoelectric materials because they are composed of both ionic and covalent bonding, which can be independently tuned. An efficient thermoelectric material would have regions of the structure composed of a high-mobility compound semiconductor that provides the “electron–crystal” electronic structure, interwoven (on the atomic scale) with a phonon transport inhibiting structure to act as the “phonon–glass”. The phonon–glass region would benefit from disorder and therefore would be ideal to house dopants without disrupting the electron–crystal region. The solid solution of the Zintl phase, Yb2–xEuxCdSb2, presents such an optimal structure, and here we characterize its thermoelectric properties above room temperature. Thermoelectric property measurements from 348 to 523 K show high Seebeck values (maximum of ~269 μV/K at 523 K) with exceptionally low thermal conductivity (minimum ~0.26 W/m K at 473 K) measured via laser flash analysis. Speed of sound data provide additional support for the low thermal conductivity. Density functional theory (DFT) was employed to determine the electronic structure and transport properties of Yb2CdSb2 and YbEuCdSb2. Lanthanide compounds display an f-band well below (~2 eV) the gap. This energy separation implies that f-orbitals are a silent player in thermoelectric properties; however, we find that some hybridization extends tomore »
- Authors:
-
[2];
[1]
- Department of Chemistry, University of California, One Shields Avenue, Davis, California 95616, United States
- Department of Chemistry, University of California, One Shields Avenue, Davis, California 95616, United States, IKERBASQUE, Basque Foundation for Science, E-48011 Bilbao, Spain
- Department of Physics, University of California, One Shields Avenue, Davis, California 95616, United States
- Department of Physics, Colorado School of Mines, Golden, Colorado 80401, United States
- Publication Date:
- Research Org.:
- Univ. of California, Davis, CA (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- Contributing Org.:
- National Energy Research Scientific Computing Center
- OSTI Identifier:
- 1416091
- Alternate Identifier(s):
- OSTI ID: 1508301; OSTI ID: 1753986
- Grant/Contract Number:
- AC02-05CH11231; NA0002908
- Resource Type:
- Published Article
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Name: Chemistry of Materials Journal Volume: 30 Journal Issue: 2; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Cooley, Joya A., Promkhan, Phichit, Gangopadhyay, Shruba, Donadio, Davide, Pickett, Warren E., Ortiz, Brenden R., Toberer, Eric S., and Kauzlarich, Susan M. High Seebeck Coefficient and Unusually Low Thermal Conductivity Near Ambient Temperatures in Layered Compound Yb 2– x Eu x CdSb 2. United States: N. p., 2017.
Web. doi:10.1021/acs.chemmater.7b04517.
Cooley, Joya A., Promkhan, Phichit, Gangopadhyay, Shruba, Donadio, Davide, Pickett, Warren E., Ortiz, Brenden R., Toberer, Eric S., & Kauzlarich, Susan M. High Seebeck Coefficient and Unusually Low Thermal Conductivity Near Ambient Temperatures in Layered Compound Yb 2– x Eu x CdSb 2. United States. https://doi.org/10.1021/acs.chemmater.7b04517
Cooley, Joya A., Promkhan, Phichit, Gangopadhyay, Shruba, Donadio, Davide, Pickett, Warren E., Ortiz, Brenden R., Toberer, Eric S., and Kauzlarich, Susan M. Mon .
"High Seebeck Coefficient and Unusually Low Thermal Conductivity Near Ambient Temperatures in Layered Compound Yb 2– x Eu x CdSb 2". United States. https://doi.org/10.1021/acs.chemmater.7b04517.
@article{osti_1416091,
title = {High Seebeck Coefficient and Unusually Low Thermal Conductivity Near Ambient Temperatures in Layered Compound Yb 2– x Eu x CdSb 2},
author = {Cooley, Joya A. and Promkhan, Phichit and Gangopadhyay, Shruba and Donadio, Davide and Pickett, Warren E. and Ortiz, Brenden R. and Toberer, Eric S. and Kauzlarich, Susan M.},
abstractNote = {Zintl phases are promising thermoelectric materials because they are composed of both ionic and covalent bonding, which can be independently tuned. An efficient thermoelectric material would have regions of the structure composed of a high-mobility compound semiconductor that provides the “electron–crystal” electronic structure, interwoven (on the atomic scale) with a phonon transport inhibiting structure to act as the “phonon–glass”. The phonon–glass region would benefit from disorder and therefore would be ideal to house dopants without disrupting the electron–crystal region. The solid solution of the Zintl phase, Yb2–xEuxCdSb2, presents such an optimal structure, and here we characterize its thermoelectric properties above room temperature. Thermoelectric property measurements from 348 to 523 K show high Seebeck values (maximum of ~269 μV/K at 523 K) with exceptionally low thermal conductivity (minimum ~0.26 W/m K at 473 K) measured via laser flash analysis. Speed of sound data provide additional support for the low thermal conductivity. Density functional theory (DFT) was employed to determine the electronic structure and transport properties of Yb2CdSb2 and YbEuCdSb2. Lanthanide compounds display an f-band well below (~2 eV) the gap. This energy separation implies that f-orbitals are a silent player in thermoelectric properties; however, we find that some hybridization extends to the bottom of the gap and somewhat renormalizes hole carrier properties. Changes in the carrier concentration related to the introduction of Eu lead to higher resistivity. A zT of ~0.67 at 523 K is demonstrated for Yb1.6Eu0.4CdSb2 due to its high Seebeck, moderate electrical resistivity, and very low thermal conductivity.},
doi = {10.1021/acs.chemmater.7b04517},
journal = {Chemistry of Materials},
number = 2,
volume = 30,
place = {United States},
year = {Mon Dec 18 00:00:00 EST 2017},
month = {Mon Dec 18 00:00:00 EST 2017}
}
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https://doi.org/10.1021/acs.chemmater.7b04517
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Cited by: 35 works
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Figures / Tables:
Figure 1: (a) Ball-and-stick depiction of the structures of Yb2−xEuxCdSb2 with one unit cell outlined. Yb, Eu, Cd, and Sb are shown as teal, pink, purple, and tan spheres, respectively. Coordination spheres of sites: (b) Yb1, interlayer, and (c) Yb2, intralayer.
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