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Matériaux composites Si@C nanostructurés pour anodes de batterie Li-ion à haute densité d’énergie. Relations entre structure/morphologie et mécanismes de dégradation

Abstract : Performing energy storage devices need to be developed in the context of Energy transition. Such systems have to maintain high energy density during a large number of cycles, to meet the challenge of clean transportation. Silicon (Si) is a good candidate for Li-ion systems anodes’ with its capacity which is 10 times higher than commercial graphite. However, silicon degradation mechanisms impede wide commercial deployment. The objective of this work is to optimize characteristics of Si to obtain performing anodes. Two strategies are employed to achieve this goal: the size reduction of Si particles and the deposition of a carbon coating on the silicon surface. The synthesis technique in this work is double stage laser pyrolysis which allows the tunable synthesis of nanoparticles. A wide range of nanoparticles, with diameters from 29 nm to 107 nm, is obtained and the best trade-off on performance is obtained for 53 nm particles. Nanoparticles with core@shell morphology (Si@C), with 29 nm diameter are obtained in one-step, the carbon representing 19 % of the total mass. The carbon coating allows a better capacity retention as 81 % of the capacity is conserved for Si@C compared to 72 % of the capacity conserved for Si particles. A fundamental study by EIS and XPS enlightens the role of the more organic chemical composition of the interphase between the solid and the electrolyte for the stabilization of the Si@C particles. Another strategy for stabilization is the design of SiGe nanostructured alloys to take advantage of the germanium stability in anodes. Several alloy compositions have been synthetized by laser pyrolysis. All alloy composition exhibit an original SiGe@Si core-shell structure which may explain the better performance obtained, compared with the state of the art.
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Antoine Desrues. Matériaux composites Si@C nanostructurés pour anodes de batterie Li-ion à haute densité d’énergie. Relations entre structure/morphologie et mécanismes de dégradation. Matériaux. Université Paris-Saclay, 2019. Français. ⟨NNT : 2019SACLS279⟩. ⟨tel-02614162⟩

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