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Title: Improved thermoelectric performance of n-type Ca and Ca-Ce filled skutterudites

Abstract

Thermoelectric (TE) technology for use in automotive waste heat recovery is being advanced by General Motors with support from the US Department of Energy. Skutterudites are a very promising material for this application of TE technology due to their superior mechanical properties and good TE performance. Double-filled YbxBayCo4Sb12 with ZT values around 1.1 at 750K are the best performing n-type skutterudites produced on a large scale using an economically viable approach of melt spinning (MS) in conjunction with spark plasma sintering (SPS). Another economical production method on the tons scale, the melt quench annealing (MQA) technique, has been recently claimed by Treibacher Industrie AG, further information is available [G. Rogl et al., Acta Mater. 76, 434-448 (2014)]. A possible hurdle to commercial implementation of these materials is the use of rare earths as the fillers to reduce thermal conductivity and improve the electrical transport properties. It will be shown herein that skutterudites double-filled with Ca and Ce, both of which are lower-cost fillers, display markedly different TE properties depending on whether they are produced by MQA or MS + SPS synthesis techniques. Finally, Ca and Ce double-filled skutterudites prepared by MS + SPS have TE properties that are superior tomore » the same compositions prepared by MQA and that are comparable to the best performing Yb and Ba filled materials. Furthermore, the results of this study suggest that the unusually poor transport properties of MQA Ca-filled skutterudites can be ascribed to deleterious secondary phases, which is contrary to reports in the literature attempting to explain these irregularities via band structure features.« less

Authors:
 [1];  [1];  [1];  [2];  [2];  [2];  [3];  [3]
+ Show Author Affiliations
  1. Optimal CAE, Plymouth, MI (United States)
  2. General Motors Research and Development, Warren, MI (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1265387
Alternate Identifier(s):
OSTI ID: 1226633
Grant/Contract Number:  
AC05-00OR22725; FC26-04NT42278; AC05000OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 116; Journal Issue: 24; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; 36 MATERIALS SCIENCE; skutterudite; thermoelectric

Citation Formats

Thompson, Daniel R., Liu, Chang, Ellison, Nicole D., Salvador, James R., Meyer, Martin S., Haddad, Daad B., Wang, Hsin, and Cai, W. Improved thermoelectric performance of n-type Ca and Ca-Ce filled skutterudites. United States: N. p., 2014. Web. doi:10.1063/1.4904187.
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Thompson, Daniel R., Liu, Chang, Ellison, Nicole D., Salvador, James R., Meyer, Martin S., Haddad, Daad B., Wang, Hsin, & Cai, W. Improved thermoelectric performance of n-type Ca and Ca-Ce filled skutterudites. United States. https://doi.org/10.1063/1.4904187
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Thompson, Daniel R., Liu, Chang, Ellison, Nicole D., Salvador, James R., Meyer, Martin S., Haddad, Daad B., Wang, Hsin, and Cai, W. Sun . "Improved thermoelectric performance of n-type Ca and Ca-Ce filled skutterudites". United States. https://doi.org/10.1063/1.4904187. https://www.osti.gov/servlets/purl/1265387.
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@article{osti_1265387,
title = {Improved thermoelectric performance of n-type Ca and Ca-Ce filled skutterudites},
author = {Thompson, Daniel R. and Liu, Chang and Ellison, Nicole D. and Salvador, James R. and Meyer, Martin S. and Haddad, Daad B. and Wang, Hsin and Cai, W.},
abstractNote = {Thermoelectric (TE) technology for use in automotive waste heat recovery is being advanced by General Motors with support from the US Department of Energy. Skutterudites are a very promising material for this application of TE technology due to their superior mechanical properties and good TE performance. Double-filled YbxBayCo4Sb12 with ZT values around 1.1 at 750K are the best performing n-type skutterudites produced on a large scale using an economically viable approach of melt spinning (MS) in conjunction with spark plasma sintering (SPS). Another economical production method on the tons scale, the melt quench annealing (MQA) technique, has been recently claimed by Treibacher Industrie AG, further information is available [G. Rogl et al., Acta Mater. 76, 434-448 (2014)]. A possible hurdle to commercial implementation of these materials is the use of rare earths as the fillers to reduce thermal conductivity and improve the electrical transport properties. It will be shown herein that skutterudites double-filled with Ca and Ce, both of which are lower-cost fillers, display markedly different TE properties depending on whether they are produced by MQA or MS + SPS synthesis techniques. Finally, Ca and Ce double-filled skutterudites prepared by MS + SPS have TE properties that are superior to the same compositions prepared by MQA and that are comparable to the best performing Yb and Ba filled materials. Furthermore, the results of this study suggest that the unusually poor transport properties of MQA Ca-filled skutterudites can be ascribed to deleterious secondary phases, which is contrary to reports in the literature attempting to explain these irregularities via band structure features.},
doi = {10.1063/1.4904187},
journal = {Journal of Applied Physics},
number = 24,
volume = 116,
place = {United States},
year = {Sun Dec 28 00:00:00 EST 2014},
month = {Sun Dec 28 00:00:00 EST 2014}
}
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https://doi.org/10.1063/1.4904187
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