SUMMARY

The development of environmentally sustainable and cheaper alternatives to conventional inorganic materials used in ion batteries is critical for addressing both resource limitations and the environmental impact of battery production. To that end, this dissertation investigates the development of electrochemically active organic materials, which offer the potential for improved sustainability, cost-effectiveness, and fine-tuned performance. This work combines multiscale atomistic modeling and machine learning to develope a framework for the molecular design of organics which exhibit enhanced alkali-ion storage capabilities. A computational framework integrating quantum mechanical calculations and machine learning is developed to facilitate the large-scale identification of novel organic materials with tailored electrochemical properties. Insights gained from this framework guide the design of carbon quantum dots exhibiting enhanced alkali-ion storage capabilities through the modulation of their functional group composition. The dissertation also investigates temperature-dependent reaction mechanisms in glyme electrolytes in CO2-containing Li-O2 batteries, offering insights into how temperature affects their stability and reactivity. Further, this work extends to investigating strategies to prolonging the cycling stability of organic cathode materials. Specifically, to inhibit the dissolution of organic cathodes in the electrolyte, this dissertation explores the development of novel solid polymer electrolytes. Employing molecular dynamics simulations with high-accuracy forcefields derived from quantum mechanical calculations, the effect of molecular design on nanophase morphology and ion transport are investigated. This aims to establish design principles for optimizing polymer electrolytes for enhanced performance and battery stability.