By yielding negative adsorption energies, our DFT calculations suggest the potential presence of fully solvated contact and solvent-separated ion pairs in close proximity to the graphite surface (see Fig. , panels a and c). However, the proximity of both these structures to the surface will likely result in the partial loss of their solvation shells and their direct adsorption onto the graphite surface, thus achieving higher energetic stability, as evidenced by ∆𝐸 ",% < 0 (see Fig. , panels b and d). This suggests a low probability of finding water within the first layer directly covering the surface, though some water molecules might be present in subsequent layers, participating in the solvation shells of the adsorbed ions. Nevertheless, the interfacial region is predicted to primarily consist of large aggregates, which could enhance overall energetic stability during their adsorption onto the graphite surface, as evidenced by the large adsorption energies of Na2OTF and NaOTF2 structures (see Fig. ).