High Potential Redox Couples: Design Strategies for Survival in Diverse Environments

Despite the numerous applications in which radical cations are used directly or as fleeting intermediates, progress in developing new materials is hindered due to the limited understanding of factors leading to stable oxidized states. Through the proposed research, we intend to develop robust electro-active materials with stable radical cations, particularly high potential redox couples, and to extend the environments in which these species can be utilized. The major scientific outcome will be a greater understanding of the behavior of these electron-deficient species in solution and in the solid state, pushing the boundaries of previously-identified structural motifs with improved stability to access higher oxidation-potential species for overcharge protection of in lithium-ion batteries and to target applications with requirements for even longer radical cation lifetimes, allowing for their use in applications beyond those in our previous studies, including as electrochemically-mediated organic transformations and polymerizations. In tandem, we will elucidate reaction mechanisms of radical cations to lead to a greater understanding of the stability and decomposition pathways of these electron-deficient species.