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Water participates actively in a wide range of interfacial adsorption and reaction processes, and its structure, dynamics, and stability, all of which are crucial to these processes, have been addressed in the present study by means of molecular dynamics simulations. The structure and dynamic behaviors of interfacial water are distinct from those of bulk water and rely strongly on the amounts of surface charges in clay minerals; for example, H-bonds exist predominately among the interfacial water molecules for zero and low surface charges, whereas prevail between the water molecules and clay surfaces for high surface charges. Stabilities of the interfacial water molecules oscillate remarkably during an increase of surface charges that first decline and then are pronouncedly enhanced. Surface charges play a critical role during the interfacial clay/water interaction, and the interfacial water molecules are "liquid-like" at zero and low surface charges but "ice-like" at high surface charges. The present results greatly promote our understanding of clays/water interfaces that exist ubiquitously in environmental conditions.

Structure, Dynamics, and Stability of Water Molecules during Interfacial Interaction with Clay Minerals: Strong Dependence on Surface Charges