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Synthèse et caractérisation de matériaux à base de SnTe pour la conversion d’énergie par effets thermoélectriques

Abstract : Lead telluride (PbTe) alloys are among the most efficient thermoelectric materials with a ZT of 1.0 for electricity generation applications in the mid to high temperature region where bismuth telluride (Bi2Te3) can no longer be used. Despite their excellent environmental stability, the perceived toxicity of lead chalcogenides can frustrate its development and large-scale application. Tin telluride (SnTe), studied more than 40 years ago as a analogue of PbTe shows poor thermoelectric performances because of its lower Seebeck coefficient. The latter is due to heavy intrinsic doping arising from spontaneous Sn vacancies. However, recent studies unambiguously show that SnTe has a strong potential of being a promising thermoelectric at high temperatures. In fact, regardless of the synthesis method used, SnTe compound is in deviation from the ideal stoichiometry (Sn vacancies). In this work, we unveil the influence of this deviation (chemical composition) and of the synthesis conditions (with quenching, without quenching, annealing and melt-spinning) on the electrical and thermal transport properties of these materials. Hence, for the synthesis of these materials different powder metallurgy techniques were implemented. The resulting materials were then finely characterized by structural and physico-chemical point of view. Thus, a detailed study of their crystalline structure was carried on by combining X-ray powder diffraction, scanning and transmission electron microscopy analyzes. The electrical and thermal properties measurements were effectuated at low temperatures (5 - 300 K) to identify the microscopic mechanisms that govern transport and at high temperatures (300 - 800 K) to determine the optimal domain of application. These measurements have confirmed the strong potential of these compounds for electricity generation applications at high temperatures. Numerous substitution possibilities at the tin and / or tellurium site have been undertaken in an attempt to further optimize the thermoelectric performance of these compounds. Substitute elements were chosen to increase the thermoelectric power through the decrease in the hole concentration or by engineering the band structure and / or decrease the lattice thermal conductivity via the formation of solid solutions or precipitates in the matrix. The choice of these elements was guided by electronic band structure calculations (DOS). The experimental results were modeled by a non-degenerate two-band model to reveal the main factors that govern the electronic transport. The lattice thermal conductivity was analyzed using the Callaway model to study the phonon scattering mechanisms at low temperatures and to better understand the influence of Sn vacancies on the thermal transport
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Submitted on : Wednesday, October 2, 2019 - 9:28:00 AM
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Dorra Ibrahim. Synthèse et caractérisation de matériaux à base de SnTe pour la conversion d’énergie par effets thermoélectriques. Matériaux. Université de Lorraine, 2018. Français. ⟨NNT : 2018LORR0137⟩. ⟨tel-01921248⟩



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