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Ion-Specific and pH-Dependent Hydration of Mica-Electrolyte Interfaces

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Grotz,  Kara K.
Emmy Noether Research Group, Department of Theoretical Biophysics, Max Planck Institute of Biophysics, Max Planck Society;

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Schwierz,  Nadine
Emmy Noether Research Group, Department of Theoretical Biophysics, Max Planck Institute of Biophysics, Max Planck Society;

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Citation

van Lin, S. R., Grotz, K. K., Siretanu, I., Schwierz, N., & Mugele, F. (2019). Ion-Specific and pH-Dependent Hydration of Mica-Electrolyte Interfaces. Langmuir, 35(17), 5737-5745. doi:10.1021/acs.langmuir.9b00520.


Cite as: http://hdl.handle.net/21.11116/0000-0003-847C-D
Abstract
Hydration forces play a crucial role in a wide range of phenomena in physics, chemistry, and biology. Here, we study the hydration of mica surfaces in contact with various alkali chloride solutions over a wide range of concentrations and pH values. Using atomic force microscopy and molecular dynamics simulations, we demonstrate that hydration forces consist of a superposition of a monotonically decaying and an oscillatory part, each with a unique dependence on the specific type of cation. The monotonic hydration force gradually decreases in strength with decreasing bulk hydration energy, leading to a transition from an overall repulsive (Li+, Na+) to an attractive (Rb+, Cs+) force. The oscillatory part, in contrast, displays a binary character, being hardly affected by the presence of strongly hydrated cations (Li+, Na+), but it becomes completely suppressed in the presence of weakly hydrated cations (Rb+, Cs+), in agreement with a less pronounced water structure in simulations. For both aspects, K+ plays an intermediate role, and decreasing pH follows the trend of increasing Rb+ and Cs+ concentrations.