Abstract
Due to their high theoretical capacity, Li-air batteries (LABs) have been considered as promising energy storage devices since their invention. However, the high complexity of these devices has impeded their practical application. Moreover, the scattered experimental results and mechanistic theories reported in literature, add difficulties to develop a comprehensive understanding of their operation principles. The work accomplished in this thesis constitutes an effort to entangle the complexity of LABs through the combination of modeling approaches with experiments, with the focus on getting better understanding about the mechanisms interplays, rather than pursuing a perfect quantitative match between simulation and experimental results. Based on continuum approach, a discharge model has been developed combining the nucleation theory, reaction kinetics and mass transport. This model converged the impacts of current density, electrolyte property and electrode surface property on the discharge process of LABs to a comprehensive theory. Furthermore, a charge model has been developed to address the important role of Li2O2 particle size distribution in determining the shape of recharge profile. In addition, to investigate the LAB system at mesoscale, a kinetic Monte Carlo (KMC) model has been build and the simulation results provided insights into the discharge process in confined environment at local level