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Synthesis and Characterization of Vacancy-Doped Neodymium Telluride for Thermoelectric Applications

Gomez, Steven J. and Cheikh, Dean and Vo, Trinh and von Allmen, Paul and Lee, Kathleen and Wood, Max and Snyder, G. Jeffrey and Dunn, Bruce S. and Fleurial, Jean-Pierre and Bux, Sabah K. (2019) Synthesis and Characterization of Vacancy-Doped Neodymium Telluride for Thermoelectric Applications. Chemistry of Materials, 31 (12). pp. 4460-4468. ISSN 0897-4756. https://resolver.caltech.edu/CaltechAUTHORS:20190611-093651432

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Abstract

Thermoelectric materials exhibit a voltage under an applied thermal gradient and are the heart of radioisotope thermoelectric generators (RTGs), which are the main power system for space missions such as Voyager I, Voyager II, and the Mars Curiosity rover. However, materials currently in use enable only modest thermal-to-electrical conversion efficiencies near 6.5% at the system level, warranting the development of material systems with improved thermoelectric performance. Previous work has demonstrated large thermoelectric figures of merit for lanthanum telluride (La_(3–x)Te_4), a high-temperature n-type material, achieving a peak zT value of 1.1 at 1275 K at an optimum cation vacancy concentration. Here, we present an investigation of the thermoelectric properties of neodymium telluride (Nd_(3–x)Te_4), another rare-earth telluride with a structure similar to La_(3–x)Te_4. Density functional theory (DFT) calculations predicted a significant increase in the Seebeck coefficient over La_(3–x)Te_4 at equivalent vacancy concentrations because of an increased density of states (DOS) near the Fermi level from the 4f electrons of Nd. The high-temperature electrical resistivity, Seebeck coefficient, and thermal conductivity were measured for Nd_(3–x)Te_4 at various carrier concentrations. These measurements were compared to La_(3–x)Te_4 in order to elucidate the impact of the four 4f electrons of Nd on the transport properties of Nd_(3–x)Te_4. A zT of 1.2 was achieved at 1273 K for Nd_(2.78)Te_4, which is a 10% improvement over that of La_(2.74)Te_4.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.chemmater.9b00964DOIArticle
ORCID:
AuthorORCID
Gomez, Steven J.0000-0002-5783-1126
Wood, Max0000-0003-2758-6155
Snyder, G. Jeffrey0000-0003-1414-8682
Dunn, Bruce S.0000-0001-5669-4740
Bux, Sabah K.0000-0002-5372-354X
Additional Information:© 2019 American Chemical Society. Received: March 8, 2019; Revised: May 15, 2019. Publication Date: June 11, 2019. The authors would like to extend special thanks to Greg Gerig and George Nakatsukasa for their aid with high-temperature measurements. Additionally, we would like to thank Chi Ma at the California Institute of Technology for his assistance performing EPMA. This work was performed at the California Institute of Technology/Jet Propulsion Laboratory under contract with the National Aeronautics and Space Administration and was supported by the NASA Science Missions Directorate’s Radioisotope Power Systems Program. The project is based upon work supported by the National Science Foundation under grant 1102531 awarded to H. Gillman, and was also supported by the National Institute of General Medical Sciences of the National Institutes of Health under award number R25GM055052 awarded to T. Hasson. The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health. The work was also supported by Caltech Summer Undergraduate Research Fellowship. Author Contributions: S.J.G. and D.C. contributed equally to this work. The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
NASA/JPL/CaltechUNSPECIFIED
NSFHRD-1102531
NIHR25GM055052
Caltech Summer Undergraduate Research Fellowship (SURF)UNSPECIFIED
Issue or Number:12
Record Number:CaltechAUTHORS:20190611-093651432
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20190611-093651432
Official Citation:Synthesis and Characterization of Vacancy-Doped Neodymium Telluride for Thermoelectric Applications. Steven J. Gomez, Dean Cheikh, Trinh Vo, Paul Von Allmen, Kathleen Lee, Max Wood, G. Jeff Snyder, Bruce S. Dunn, Jean-Pierre Fleurial, and Sabah K. Bux. Chemistry of Materials 2019 31 (12), 4460-4468 DOI: 10.1021/acs.chemmater.9b00964
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:96271
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:11 Jun 2019 16:49
Last Modified:03 Oct 2019 21:20

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