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Title: High thermoelectric performance of In, Yb, Ce multiple filled CoSb{sub 3} based skutterudite compounds

Abstract

Filling voids with rare earth atoms is an effective way to lowering thermal conductivity which necessarily enhances thermoelectric properties of skutterudite compounds. Yb atom is one of the most effective species among the rare earth atoms for filling the voids in the skutterudite structure due to a large atomic mass, radius and it is intermediate valence state. In this work, we aim to find the best filling partners for Yb using different combinations of Ce and In as well as to optimize actual filling fraction in order to achieve high values of ZT. The traditional method of synthesis relying on melting-annealing and followed by spark plasma sintering was used to prepare all samples. The thermoelectric properties of four samples of Yb{sub 0.2}In{sub 0.2}Co{sub 4}Sb{sub 12}, Yb{sub 0.2}Ce{sub 0.15}Co{sub 4}Sb{sub 12}, Yb{sub 0.2}Ce{sub 0.15}In{sub 0.2}Co{sub 4}Sb{sub 12}, and Yb{sub 0.3}Ce{sub 0.15}In{sub 0.2}Co{sub 4}Sb{sub 12} (nominal) were examined based on the Seebeck coefficient, electrical conductivity, thermal conductivity, and Hall coefficient. Hall coefficient and Seebeck coefficient signs confirm that all samples are n-type skutterudite compounds. Carrier density increases with the increasing Yb+Ce content. A high power factor value of 57.7 {mu}W/K{sup 2}/cm for Yb{sub 0.2}Ce{sub 0.15}Co{sub 4}Sb{sub 12} and a lower thermal conductivitymore » value of 2.82 W/m/K for Yb{sub 0.2}Ce{sub 0.15}In{sub 0.2}Co{sub 4}Sb{sub 12} indicate that small quantities of Ce with In may be a good partner to Yb to reduce the thermal conductivity further and thus enhance the thermoelectric performance of skutterudites. The highest ZT value of 1.43 was achieved for Yb{sub 0.2}Ce{sub 0.15}In{sub 0.2}Co{sub 4}Sb{sub 12} triple-filled skutterudite at 800 K. - Graphical abstract: Thermoelectric figure of merit of Yb{sub x}In{sub y}Ce{sub z}Co{sub 4}Sb{sub 12} (0{<=}x,y,z{<=}0.18 actual) compounds versus temperature. Highlights: Black-Right-Pointing-Pointer TE properties of Yb,In,Ce multiple-filled Yb{sub x}In{sub y}Ce{sub z}Co{sub 4}Sb{sub 12} skutterudites were investigated. Black-Right-Pointing-Pointer Thermal conductivity is strongly suppressed by multiple filling of Yb, Ce and In. Black-Right-Pointing-Pointer Small amounts of Ce and In with Yb are beneficial for the enhancement of TE performance. Black-Right-Pointing-Pointer The highest ZT=1.43 was achieved with Yb{sub 0.07}In{sub 0.094}Ce{sub 0.065}Co{sub 4}Sb{sub 11.92} at 800 K.« less

Authors:
 [1]; ;  [1];  [2];  [3]
  1. Department of Physics, University of Istanbul, 34134 Vezneciler, Istanbul (Turkey)
  2. Chemical Sci. and Mater. Systems Laboratory, General Motors Global R and D Center, Warren, MI 48090 (United States)
  3. Department of Physics, University of Michigan, Ann Arbor, MI, 48109 (United States)
Publication Date:
OSTI Identifier:
22149796
Resource Type:
Journal Article
Journal Name:
Journal of Solid State Chemistry
Additional Journal Information:
Journal Volume: 193; Other Information: Copyright (c) 2012 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0022-4596
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CARRIER DENSITY; COBALT SULFIDES; ELECTRIC CONDUCTIVITY; RARE EARTHS; SYNTHESIS; THERMAL CONDUCTIVITY; THERMOELECTRIC PROPERTIES

Citation Formats

Ballikaya, Sedat, Department of Physics, University of Michigan, Ann Arbor, MI, 48109, Uzar, Neslihan, Yildirim, Saffettin, Salvador, James R., and Uher, Ctirad. High thermoelectric performance of In, Yb, Ce multiple filled CoSb{sub 3} based skutterudite compounds. United States: N. p., 2012. Web. doi:10.1016/J.JSSC.2012.03.029.
Ballikaya, Sedat, Department of Physics, University of Michigan, Ann Arbor, MI, 48109, Uzar, Neslihan, Yildirim, Saffettin, Salvador, James R., & Uher, Ctirad. High thermoelectric performance of In, Yb, Ce multiple filled CoSb{sub 3} based skutterudite compounds. United States. https://doi.org/10.1016/J.JSSC.2012.03.029
Ballikaya, Sedat, Department of Physics, University of Michigan, Ann Arbor, MI, 48109, Uzar, Neslihan, Yildirim, Saffettin, Salvador, James R., and Uher, Ctirad. Sat . "High thermoelectric performance of In, Yb, Ce multiple filled CoSb{sub 3} based skutterudite compounds". United States. https://doi.org/10.1016/J.JSSC.2012.03.029.
@article{osti_22149796,
title = {High thermoelectric performance of In, Yb, Ce multiple filled CoSb{sub 3} based skutterudite compounds},
author = {Ballikaya, Sedat and Department of Physics, University of Michigan, Ann Arbor, MI, 48109 and Uzar, Neslihan and Yildirim, Saffettin and Salvador, James R. and Uher, Ctirad},
abstractNote = {Filling voids with rare earth atoms is an effective way to lowering thermal conductivity which necessarily enhances thermoelectric properties of skutterudite compounds. Yb atom is one of the most effective species among the rare earth atoms for filling the voids in the skutterudite structure due to a large atomic mass, radius and it is intermediate valence state. In this work, we aim to find the best filling partners for Yb using different combinations of Ce and In as well as to optimize actual filling fraction in order to achieve high values of ZT. The traditional method of synthesis relying on melting-annealing and followed by spark plasma sintering was used to prepare all samples. The thermoelectric properties of four samples of Yb{sub 0.2}In{sub 0.2}Co{sub 4}Sb{sub 12}, Yb{sub 0.2}Ce{sub 0.15}Co{sub 4}Sb{sub 12}, Yb{sub 0.2}Ce{sub 0.15}In{sub 0.2}Co{sub 4}Sb{sub 12}, and Yb{sub 0.3}Ce{sub 0.15}In{sub 0.2}Co{sub 4}Sb{sub 12} (nominal) were examined based on the Seebeck coefficient, electrical conductivity, thermal conductivity, and Hall coefficient. Hall coefficient and Seebeck coefficient signs confirm that all samples are n-type skutterudite compounds. Carrier density increases with the increasing Yb+Ce content. A high power factor value of 57.7 {mu}W/K{sup 2}/cm for Yb{sub 0.2}Ce{sub 0.15}Co{sub 4}Sb{sub 12} and a lower thermal conductivity value of 2.82 W/m/K for Yb{sub 0.2}Ce{sub 0.15}In{sub 0.2}Co{sub 4}Sb{sub 12} indicate that small quantities of Ce with In may be a good partner to Yb to reduce the thermal conductivity further and thus enhance the thermoelectric performance of skutterudites. The highest ZT value of 1.43 was achieved for Yb{sub 0.2}Ce{sub 0.15}In{sub 0.2}Co{sub 4}Sb{sub 12} triple-filled skutterudite at 800 K. - Graphical abstract: Thermoelectric figure of merit of Yb{sub x}In{sub y}Ce{sub z}Co{sub 4}Sb{sub 12} (0{<=}x,y,z{<=}0.18 actual) compounds versus temperature. Highlights: Black-Right-Pointing-Pointer TE properties of Yb,In,Ce multiple-filled Yb{sub x}In{sub y}Ce{sub z}Co{sub 4}Sb{sub 12} skutterudites were investigated. Black-Right-Pointing-Pointer Thermal conductivity is strongly suppressed by multiple filling of Yb, Ce and In. Black-Right-Pointing-Pointer Small amounts of Ce and In with Yb are beneficial for the enhancement of TE performance. Black-Right-Pointing-Pointer The highest ZT=1.43 was achieved with Yb{sub 0.07}In{sub 0.094}Ce{sub 0.065}Co{sub 4}Sb{sub 11.92} at 800 K.},
doi = {10.1016/J.JSSC.2012.03.029},
url = {https://www.osti.gov/biblio/22149796}, journal = {Journal of Solid State Chemistry},
issn = {0022-4596},
number = ,
volume = 193,
place = {United States},
year = {2012},
month = {9}
}