The optical, electronic, and mechanical properties of graphite, few-layer, and two-dimensional (2D) materials have prompted a considerable number of applications. Biosensing, energy storage, and water desalination illustrate applications that require a molecular-scale understanding of the interfacial water structure on 2D materials. This review introduces the most recent experimental and theoretical advances on the structure of interfacial liquid water on graphite-like and 2D materials surfaces. On pristine conditions, atomic-scale resolution experiments revealed the existence of 1-3 hydration layers. Those layers were separated by ∼0.3 nm. The experimental data were supported by molecular dynamics simulations. However, under standard working conditions, atomic-scale resolution experiments revealed the presence of 2-3 hydrocarbon layers. Those layers were separated by ∼0.5 nm. Linear alkanes were the dominant molecular specie within the hydrocarbon layers. Paradoxically, the interface of an aged 2D material surface immersed in water does not have water molecules on its vicinity. Free-energy considerations favored the replacement of water by alkanes.
Keywords: 2D materials-water interfaces; AFM; WCA; airborne contaminants; graphite−water interfaces; interfacial water; molecular dynamics simulations; solid−liquid interfaces; three-dimensional AFM.