The role of the water contact layer on hydration and transport at solid/liquid interfaces.

Autor:	Gäding J; Institute of Soft Matter Modeling, Hamburg University of Technology, Hamburg 21073, Germany.; Institute of Surface Science, Department of Atomistic Corrosion Informatics, Helmholtz-Zentrum Hereon, Geesthacht 21502, Germany., Della Balda V; Department of Chemistry, University of Zurich, Zurich 8057, Switzerland., Lan J; Department of Chemistry, New York University, New York, NY 10003.; Department of Chemistry, Simons Center for Computational Physical Chemistry at New York University, New York, NY 10003., Konrad J; Institute of Soft Matter Modeling, Hamburg University of Technology, Hamburg 21073, Germany., Iannuzzi M; Department of Chemistry, University of Zurich, Zurich 8057, Switzerland., Meißner RH; Institute of Soft Matter Modeling, Hamburg University of Technology, Hamburg 21073, Germany.; Institute of Surface Science, Department of Atomistic Corrosion Informatics, Helmholtz-Zentrum Hereon, Geesthacht 21502, Germany., Tocci G; Department of Chemistry, University of Zurich, Zurich 8057, Switzerland.
Jazyk:	angličtina
Zdroj:	Proceedings of the National Academy of Sciences of the United States of America [Proc Natl Acad Sci U S A] 2024 Sep 17; Vol. 121 (38), pp. e2407877121. Date of Electronic Publication: 2024 Sep 11.
DOI:	10.1073/pnas.2407877121
Abstrakt:	Understanding the structure in the nanoscopic region of water that is in direct contact with solid surfaces, so-called contact layer, is key to quantifying macroscopic properties that are of interest to e.g. catalysis, ice nucleation, nanofluidics, gas adsorption, and sensing. We explore the structure of the water contact layer on various technologically relevant solid surfaces, namely graphene, MoS[Formula: see text], Au(111), Au(100), Pt(111), and Pt(100), which have been previously hampered by time and length scale limitations of ab initio approaches or force field inaccuracies, by means of molecular dynamics simulations based on ab initio machine learning potentials built using an active learning scheme. Our results reveal that the in-plane intermolecular correlations of the water contact layer vary greatly among different systems: Whereas the contact layer on graphene and on Au(111) is predominantly homogeneous and isotropic, it is inhomogeneous and anisotropic on MoS[Formula: see text], on Au(100), and on the Pt surfaces, where it additionally forms two distinct sublayers. We apply hydrodynamics and the theory of the hydrophobic effect, to relate the energy corrugation and the characteristic length-scales of the contact layer with wetting, slippage, the hydration of small hydrophobic solutes and diffusio-osmotic transport. Thus, this work provides a microscopic picture of the water contact layer and links it to macroscopic properties of liquid/solid interfaces that are measured experimentally and that are relevant to wetting, hydrophobic solvation, nanofluidics, and osmotic transport. Competing Interests: Competing interests statement:The authors declare no competing interest.
Databáze:	MEDLINE
Externí odkaz:	Zobrazit plný text záznamu