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Through molecular dynamics simulations considering thermal vibration ofsurface atoms, ionic behaviors in concentrated NaCl solutions confined betweendiscretely charged silicon surfaces have been investigated. The electric doublelayer structure was found sensitive to the density and distribution of surfacecharges. Due to the surface charge discreteness, slight charge inversionappeared which depended on the surface charge density, bulk concentration andconfinement. In the nanoconfined NaCl solutions differently concentrated from0.2 M to 4.0 M, the locations of accumulation layers for Na+ and Cl- ions keptstable, but their peak values increased. The higher the concentration was, themore obvious charge inversion appeared. In 4.0 M NaCl solution, Na+ and Cl-ions show obvious alternating layered distributions which may be correspondingto the solidification found in experiments. By changing surface separation, theconfinement had a large effect on ionic distributions. As both surfacesapproached each other, many ions and water molecules were squeezed out of theconfined space. Two adjacent layers in ion or water distribution profiles canbe forced to closer to each other and merge together. From ionic hydrationanalysis, the coordination number of Na+ ions in highly-confined space was muchlower than that in the bulk.

Ionic Behavior in Highly Concentrated Aqueous Solutions Nanoconfined between Discretely Charged Silicon Surfaces