Superhydrophilicity of ?-alumina surfaces results from tight binding of interfacial waters to specific aluminols br

Hypothesis: Understanding the microscopic driving force of water wetting is challenging and important for design of materials. The relations between structure, dynamics and hydrogen bonds of interfacial water can be investigated using molecular dynamics simulations.Experiments and simulations: Contact angles at the alumina (0001) and (1120) surfaces are studied using both classical molecular dynamics simulations and experiments. To test the superhydrophilicity, the free energy cost of removing waters near the interfaces are calculated using the density fluctuations method. The strength of hydrogen bonds is determined by their lifetime and geometry.Findings: Both surfaces are superhydrophilic and the (0001) surface is more hydrophilic. Interactions between surfaces and interfacial waters promote a templating effect whereby the latter are aligned in a pattern that follows the underlying lattice of the surfaces. Translational and rotational dynamics of interfacial water molecules are slower than in bulk water. Hydrogen bonds between water and both sur-faces are asymmetric, water-to-aluminol ones are stronger than aluminol-to-water ones. Molecular dynamics simulations eliminate the impacts of surface contamination when measuring contact angles and the results reveal the microscopic origin of the macroscopic superhydrophilicity of alumina surfaces: strong water-to-aluminol hydrogen bonds. (c) 2022 Published by Elsevier Inc.

Automated summary

Understanding the microscopic driving force of water wetting is challenging and important for material design. This study investigates the relations between structure, dynamics and hydrogen bonds of interfacial water on alumina surfaces using molecular dynamics simulations and experiments. The findings reveal superhydrophilicity of both surfaces, with the (0001) surface being more hydrophilic. The molecular dynamics simulations eliminate surface contamination and provide insights into the microscopic origin of the macroscopic superhydrophilicity: strong water-to-aluminol hydrogen bonds.