Ionic liquids (ILs) have garnered immense attention due to their tunable physicochemical properties. In this study, we delve into the wetting behaviour and interfacial properties of aqueous binary IL mixtures containing [EMIM] [BF4] and [HMIM] [BF4] on both smooth and rough graphite surfaces. Employing classical molecular dynamics simulations, we systematically explored the effects of IL concentration and surface morphology on wetting phenomena. To ensure the equilibrium of the systems, we began by calculating the interaction energies between the components. Subsequently, contact angles were computed, shedding light on the wetting characteristics of the aqueous binary IL mixtures. We meticulously examined the density profiles of the IL systems from the substrate to unravel the dominance of one IL over the other, exploiting the hydrophilic nature of [EMIM] [BF4] and the hydrophobic nature of [HMIM] [BF4]. A comprehensive analysis of hydrogen bond distribution allowed us to discern the intricate nature of these aqueous binary IL droplets. We probed the changes in intermolecular forces within the aqueous IL solution by investigating surface tensions. The tunability of these ILs emerges as a significant aspect of our study, paving the way for their tailored application in engineering and scientific domains. Schematic diagram showing the density distribution of hydrophilic and hydrophobic ILs ([EMIM] [BF4] and [HMIM] [BF4]) in water and also the hydrogen bond (HB) distribution of anion ([BF4]−) water inside the droplet on a pillared surface with a surface fraction ( f ) of 0.4 and pillar height of H = 4 .
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