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The electrolyte intercalation mechanism facilitates the insertion/extractionof charge into the electrode material in rechargeable batteries. Aluminumfluoride (AlF$_{3}$) has been used as an electrolyte in rechargeable aluminumbatteries with graphite electrodes, demonstrating improved reversibility ofbattery charging and discharging processes; however, the intercalationmechanism of this neutral molecule in graphite is so far unknown. In this work,we combine scanning tunneling microscopy (STM) in ultra-high vacuum conditions,calculations based on density functional theory, and large-scale moleculardynamics simulations to reveal the mechanism of AlF$_{3}$ intercalation inhighly oriented pyrolytic graphite (HOPG). We report the formation of AlF$_{3}$molecules clusters between graphite layers, their self-assembly by graphenebuckling-mediated interactions, and explain the origin and distribution ofsuperficial {\it blisters} in the material. Our findings have implications forunderstanding the relationship between the mobility and clustering of moleculesand the expansion of the anode material. This, in turn, paves the way forfuture enhancements in the performance of energy storage systems.

acs applied nano materials

Study of In-plane and Interlayer Interactions During Aluminum Fluoride  Intercalation in Graphite: Implications for the Development of Rechargeable  Batteries