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Contribution to improving the reliability of thermoelectric modules : development of alternative material solutions

Abstract : Energy conversion from waste heat through thermoelectric effects (Seebeck effect) is a potential new renewable energy source. The thermoelectric (TE) technology is nevertheless limited to niche terrestrial applications due to its low efficiency (5-6%), but also due to the technological challenges to be overcome to avoid a degradation of the TE generators (TEG). Our thesis is devoted to this problem within the framework of a research program supported by the ANR (RELIATEG project) including HotBlockOnBoard (HBOB), CEA LITEN, CIRIMAT and IJL as partners. The objective is to make reliable the TEG, manufactured by HBOB, based on silicides, Mg₂Si₁₋ₓSnₓ (n-type) and MnSi₁₊ᵧ (p-type), for long-term use in the vicinity of 400-500°C. Our main role is to understand the mechanisms leading to their embrittlement, particularly to the oxidation problems linked to the Mg₂Si₀,₆Sn₀,₄ material. As they are unavoidable, we turned to the solutions of finding a protective coating and/or testing the thermal stability under air of a Mg₂Si₁₋ₓSnₓ material, less sensitive to oxidation. After a bibliographical synthesis of the basic concepts of TE and of the state of the art of TE materials, the choice of materials used by HBOB have been justified. The various stages of TEG manufacturing and the experimental techniques used to characterize the microstructure of TE materials and their thermal stability are presented. The performance tests performed on TEGs show that the power obtained, measured up to 450°C, is reproducible for the 25 devices tested. However, it is about 25% lower than what one could achieve with a perfect TEG, as shown by the simulations we carried out using the Comsol MultiPhysics software. The stability tests showed that the devices are stable under air at 250°C, for 500 hours or under 1000 cycles, and that they begin to degrade under air at 350°C through a pesting phenomenon linked to the oxidation of Mg₂Si₀,₆Sn₀,₄. Under vacuum, this process is slowed down but the presence of residual oxygen does not completely stabilize the material. At 500°C under air, the pesting is observed from 3 hours of testing. The oxidation tests carried out on the two materials with different Sn content showed the significant role of tin on the oxidation phenomena. A model explaining the pesting phenomenon was developed by the combined analyses of results obtained by thermogravimetric measurements, scanning electron microscopy and X-ray diffraction. On the basis of bibliography and phase diagrams of the differents systems, protective coatings based on ceramics, metallic silicides, metals and glasses have been studied. Several deposition methods were explored: sintering by Spark Plasma Sintering, electrochemical nickel plating, pack cementation, slurry, PVD and spray deposits. The most promising coatings were obtained with a glass whose CTE is close to that of the n-type material.
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Submitted on : Wednesday, June 9, 2021 - 10:47:36 AM
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  • HAL Id : tel-03254813, version 1


Mostafa Oulfarsi. Contribution to improving the reliability of thermoelectric modules : development of alternative material solutions. Materials Science [cond-mat.mtrl-sci]. Université de Lorraine, 2020. English. ⟨NNT : 2020LORR0228⟩. ⟨tel-03254813⟩



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