(644i) Insights into Li-Ion Battery Cathode Degradation from Atomic-Scale Modeling

Interfacial reactions during cycling are one of the obstacles that prevent the commercialization of high-energy-dense Li-rich cathode materials for the next generation of Li-ion batteries. To engineer more stable cathode compositions or protective surface coatings, an understanding of the fundamental degradation processes on the atomic scale is needed. While new experimental techniques can reach high resolutions, the experimental in-situ characterization of atomic-scale processes at narrow interface regions is still challenging. Here, we show how first-principles atomistic modeling can provide insights into surface and interface reactivity that is complementary to experimental characterization. Using automated density-functional theory calculations, we map the self-reductive decomposition of Li transition-metal oxides. The observed trends can function as a guideline for the development of degradation-stable cathode compositions and improved coating materials.