Study and improvement of non-aqueous Lithium-Air batteries via the development of a silicon-based anode

Abstract : Supplying the world energy demand while reducing the greenhouse gases emissions is one of the biggest challenges of the 21st century; this requires the development of efficient energy storage devices enabling the utilization of renewable energies. Among them, Lithium-Air batteries are very attractive due to their high theoretical energy density – 10 times that of the current Li-ion batteries – but their development is hindered by the complexity of the chemistry at play. In order to understand such chemistry, we designed a new electrochemical test cell that integrates a pressure sensor, thereby enabling an accurate in operando monitoring of the pressure changes during charge/discharge with high reproducibility and sensitivity. Its use is demonstrated by quantifying the parasitic reactions in Li-O2 cells for various electrolytes frequently encountered in the literature. Through this comparative study, we are able to observe the phenomena currently limiting the performances of Li-O2 batteries after a long cycling (> 1000 h), such as parasitic reactions and the instability of the Li anode. To address the later issue, Li was replaced by a prelithiated silicon electrode made of Si particles oxidized in surface. We demonstrated the feasibility of enhancing both their capacity and cycle life via a pre-formatting treatment that triggers the reduction of their SiO2 coating by liberating pure Si metal. The full LixSi-O2 cells using such treated electrodes exhibit performances competing with the best analogous systems reported in the literature (> 30 cycles; more than 400 h of cycling), but the development of practical prototypes still requires to improve the cycle-life.
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Florent Lepoivre. Study and improvement of non-aqueous Lithium-Air batteries via the development of a silicon-based anode. Material chemistry. Université Pierre et Marie Curie - Paris VI, 2016. English. ⟨NNT : 2016PA066326⟩. ⟨tel-01474849⟩

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