Langmuir, Vol.27, No.8, 4690-4699, 2011
Water Structure and Dynamics at a Silica Surface: Pake Doublets in H-1 NMR Spectra
Detailed knowledge about the dynamics and, structure of liquids in the vicinity of 4 solid wsurface is important in several fields of research.:in this study a homogeneous model system of colloidal and nonporous silica particles with a narrow particle size distribution was used to examine such properties adsorbed-water and 1-heptanol. Doublet H-1 water resonances ("Pake doublets") indicate a preferred spatial orientation for the water molecules, as well as a lower molecular density in the surface-induced water structures compared to bulk water. These surface-induced structures are found to extend at least 8 nm from the silica surface. T-1 relaxation measurements at several temperatures indicate weaker H-bonding in the adsorbed water compared to bulk water. T-2 relaxation measurements at several temperatures reveal the presence of two water phases and give quantitative information on the mobility of water molecules and proton exchange processes. The presence of 1-heptanol changes the water characteristics, primarily in the water phase closer to the surface, where water molecules experience decreased translational and increased rotational freedom. In the absence of water, adsorbed 1-heptanol forms surface aggregates encompassing several molecular layers, where the first adsorbed layer shows severe restrictions in mobility and subsequent layers are more mobile.