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Jaumaux, Pauline
01/2022Dissertation
Greenhouse gas emission related to the burning of fossil fuels for energy production is the main driver responsible for the climate crisis our society is facing. To avert climate change, the transition toward renewable energy production is urgent. However, the intermittence of these energy sources restrict their implementation. Coupling sustainable energy sources with energy storage systems could solve this issue. Since its commercialisation, Lithium (Li) -ion batteries have been at the centre of the attention for high-energy storage systems. As the global energy demand keeps increasing, new battery requirements are expected such as higher energy density and improved safety, which cannot be met by the current commercial Li-ion batteries. The thermally instable liquid electrolyte (containing highly flammable and toxic solvents, and thermally instable Li salts) usually employed in Li-ion batteries causes serious safety concerns. Many fires and explosions incidents occurred in the past few decades due to over-heating Li-ion batteries. Herein, various non-flammable electrolytes such as deep-eutectic-solvents and aqueous electrolytes were engineered to answer safety, dendrite growth and cost issues in Li and zinc (Zn) –based batteries. A fluorinated self-healing deep eutectic solvent quasi-solid electrolyte allowed long cycling performance of a Li-metal battery (Li||lithium manganese oxide (LiMn2O4, LMO) by creating a robust protective layer on the Li anode meanwhile the gel matrix helped guiding the Li deposition, thereby reducing dendrite growth and maintaining high safety. Then, a localized highly concentrated aqueous quasi-solid electrolyte was designed for low-cost Li-ion aqueous batteries with high voltage LMO cathode. Finally, a molecular crowding strategy was employed to suppress dendrite growth and corrosion on Zn metal anode in hybrid Zn||LMO aqueous batteries. These electrolyte designs opened up fascinating ways to tailor electrolyte properties for high safety and low-cost next battery generation.
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