Publication date: 10th April 2024
Meeting the escalating energy demands of electric vehicles and portable devices necessitates high-energy rechargeable batteries. Although Li-ion batteries are prevalent, they face challenges related to energy density, charging rates, and safety concerns associated with flammable liquid electrolytes. To address these issues, researchers are exploring alternative batteries or investigating solid-state electrolytes as a safer alternative to conventional Li-ion batteries. Among various inorganic materials garnering attention in solid-state battery systems, Li-La-Ti-O (LLTO) stands out as a promising candidate as it exhibits high bulk Li ion conductivity, excellent high voltage stability, and remarkable hardness, which mitigates dendrite formation. Consequently, there have been several efforts to improve their conductivity. Literature suggests that the low conductivity of LLTO is due to grain boundaries, while conversely, LLTO conductivity increases in the presence of TiO2. Both effects, the negative impact of grain boundaries and the positive influence of TiO2 lack a satisfactory explanation, prompting us to perform a comprehensive Molecular Dynamics investigation. Our study involves a detailed analysis of symmetric and mixed LLTO grain boundaries and LLTO/TiO₂ interfaces under diverse conditions. This exploration has yielded intriguing insights into the complex interplay of these factors. In this presentation, I will share our results and delve into the intricate migration mechanisms of Li-ion within the elaborate microstructures of LLTO. These findings not only shed light on the mysterious phenomena of LLTO conductivity but also offer valuable perspectives for designing and optimizing solid-state batteries, shaping the future of energy storage applications.
The authors acknowledge the Natural Sciences and Engineering Research Council of Canada (NSERC) Discovery grant program, [Funding Reference number RGPIN-2020-05924], Canada Research Chair (CRC) program, and the Canada Foundation for Innovation (CFI) for infrastructure and operating funds. This research was enabled in part by support provided by Calcul Québec (https://www.calculquebec.ca) and the Digital Research Alliance of Canada (alliancecan.ca).
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