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A comprehensive study of the crystallization of Cu–As–Te glasses: microstructure and thermoelectric properties

Vaney, J. B. and Delaizir, G. and Alleno, E. and Rouleau, O. and Piarristeguy, A. and Monnier, J. and Godart, C. and Ribes, M. and Escalier, R. and Pradel, A. and Gonçalves, A. P. and Lopes, E. B. and Cuello, G. J. and Ziolkowski, P. and Müller, E. and Candolfi, C. and Dauscher, A. and Lenoir, B. (2013) A comprehensive study of the crystallization of Cu–As–Te glasses: microstructure and thermoelectric properties. Journal of Materials Chemistry A, 1, pp. 8190-8200. Royal Society of Chemistry. DOI: 10.1039/C3TA11159H ISSN 2050-7488

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Abstract

We report a thorough experimental study on the microstructure, thermal behavior and thermoelectric properties of the amorphous composition Cu15As30Te55 and the glass–ceramics related-compounds synthesized by using the Spark Plasma Sintering (SPS) technique. Varying the conditions of the SPS process enables the synthesis of composite glassy-crystalline samples with different crystal/glass ratios. Such treatments result in complex microstructures composed of large glassy domains where nanocrystals of the metastable β-As2Te3 phase are embedded. These domains are separated by regions of the dendritic crystalline phase surrounded by a Cu-rich glassy matrix. The presence of β-As2Te3, confirmed by both powder X-ray diffraction and scanning electron microscopy, suggests that pressure and/or internal stresses play an important role in stabilizing this phase. This conclusion is further supported by neutron thermodiffraction experiments revealing a sharp crossover from the β-As2Te3 to the stable α-As2Te3 phase at temperatures below that of the SPS treatment. Transport properties measurements show that the presence of a crystalline fraction significantly lowers the electrical resistivity by four orders of magnitude. However, the probable intrinsic n-type behavior of β-As2Te3 has a detrimental influence on the thermopower values. Even though the partial crystallization of the glassy matrix leads to an increase in the thermal conductivity, the measured values remain on the order of 1 W m−1 K−1 at 300 K. Besides an overall increase in the dimensionless figure of merit ZT, our results demonstrate that the partial crystallization of an amorphous matrix is an efficient tool to tune the electrical resistivity over several orders of magnitude while maintaining low thermal conductivity values.

Item URL in elib:https://elib.dlr.de/85833/
Document Type:Article
Title:A comprehensive study of the crystallization of Cu–As–Te glasses: microstructure and thermoelectric properties
Authors:
AuthorsInstitution or Email of AuthorsAuthors ORCID iD
Vaney, J. B. Institut Jean Lamour (IJL), UMR 7198 CNRS-Université de Lorraine, FranceUNSPECIFIED
Delaizir, G.Sciences des Procédés Céramique et de Traitement de Surface (SPCTS), UMR CNRS 7315, Centre Européen de la Céramique, Limoges, FranceUNSPECIFIED
Alleno, E.Institut de Chimie et des Matériaux de Paris Est (ICMPE), UMR 7182 CNRS, CMTR, Thiais, FranceUNSPECIFIED
Rouleau, O.Institut de Chimie et des Matériaux de Paris Est (ICMPE), UMR 7182 CNRS, CMTR, Thiais, FranceUNSPECIFIED
Piarristeguy, A.Institut Charles Gerhardt (ICG), UMR 5253 CNRS-Université Montpellier 2, FranceUNSPECIFIED
Monnier, J.Institut de Chimie et des Matériaux de Paris Est (ICMPE), UMR 7182 CNRS, CMTR, Thiais, FranceUNSPECIFIED
Godart, C.Institut de Chimie et des Matériaux de Paris Est (ICMPE), UMR 7182 CNRS, CMTR, Thiais, FranceUNSPECIFIED
Ribes, M.Institut Charles Gerhardt (ICG), UMR 5253 CNRS-Université Montpellier 2, FranceUNSPECIFIED
Escalier, R.Institut Charles Gerhardt (ICG), UMR 5253 CNRS-Université Montpellier 2, FranceUNSPECIFIED
Pradel, A.Institut Charles Gerhardt (ICG), UMR 5253 CNRS-Université Montpellier 2, FranceUNSPECIFIED
Gonçalves, A. P.ST/ITN Instituto Superior Técnico, Universidade Técnica de Lisboa, P-2686-953UNSPECIFIED
Lopes, E. B.ST/ITN Instituto Superior Técnico, Universidade Técnica de Lisboa, P-2686-953UNSPECIFIED
Cuello, G. J.Institut Laue Langevin, 6 rue Jules Horowitz, B. P. 156, 38042 Grenoble, FranceUNSPECIFIED
Ziolkowski, P.German Aerospace Center, Institute of Materials Research, Köln, GermanyUNSPECIFIED
Müller, E.German Aerospace Center, Institute of Materials Research, Köln, GermanyUNSPECIFIED
Candolfi, C.Institut Jean Lamour (IJL), UMR 7198 CNRS-Université de Lorraine, FranceUNSPECIFIED
Dauscher, A.Institut Jean Lamour (IJL), UMR 7198 CNRS-Université de Lorraine, FranceUNSPECIFIED
Lenoir, B. Institut Jean Lamour (IJL), UMR 7198 CNRS-Université de Lorraine, FranceUNSPECIFIED
Date:13 May 2013
Journal or Publication Title:Journal of Materials Chemistry A
Refereed publication:Yes
Open Access:No
Gold Open Access:No
In SCOPUS:Yes
In ISI Web of Science:Yes
Volume:1
DOI :10.1039/C3TA11159H
Page Range:pp. 8190-8200
Publisher:Royal Society of Chemistry
ISSN:2050-7488
Status:Published
Keywords:thermoelectrics; SPS; Cu-As-Te
HGF - Research field:Aeronautics, Space and Transport
HGF - Program:Aeronautics
HGF - Program Themes:Propulsion Systems (old)
DLR - Research area:Aeronautics
DLR - Program:L ER - Engine Research
DLR - Research theme (Project):L - Turbine Technologies (old)
Location: Köln-Porz
Institutes and Institutions:Institute of Materials Research > Thermoelectric Materials and Systems
Deposited By: Zabrocki, Dr. Knud
Deposited On:27 Nov 2013 14:28
Last Modified:06 Sep 2019 15:30

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