Lithium-Oxygen and Lithium-Air batteries promise high theoretical energy densities that are significantly greater than current lithium-ion technology and available from an abundant ambient resource. The advantage of such a high-energy active material that could be extracted from ambient air could help achieve the strict requirements for electric and hybrid aviation. However, the major limiting factor for adopting these systems is the high rate of degradation and side-product formation in non-aqueous electrolytes utilizing carbon cathode supports.The decomposition of organic electrolyte and carbon cathode result in poor cycling performance due to build up of intermediates, such as lithium-carbonate (Li2CO3), at the cathode surface, and resulting in poor cycle efficiency. In this study, a combined approach utilizing both computational modeling and experimental screening was used to investigate novel electrolytes and carbon-free cathode materials to reduce or avoid the generation of carbonates during cell operation.