Hybrid quantum-classical treatment of lithium ion transfer reactions at graphite-electrolyte interfaces

Ion intercalation and deintercalation (IID) reactions in rechargeable metal-ion batteries are affected by the electrochemical double layer (EDL) at solid-liquid interfaces. Yet, EDL effects on the kinetics of IID reactions are less considered. Here, we develop a hybrid quantum-classical model for IID reactions at graphite-electrolyte interfaces that accounts for the coupling of ion and electron transfer processes, and the influence of the inhomogeneous local EDL environment. The model is employed to understand how the structural deformation of the graphite electrode, the electric potential, and the solvent dipole moment shape the kinetics of IID reactions.