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For a solvent, which shows no selectivity, the two surface Pourbaix diagrams would have been identical. This is obviously not the case. In fact, the impact of the solvent is dramatic: It leads not only to a shift of the phase boundaries which would indicate that one surface profits energetically more than the other does , but also to the stabilization of surface reconstructions that are thermodynamically unstable in an ambient gas phase environment.

The left diagram, in which the effect of solvation is reduced to the chemisorption of the dissociated water fragments H and OH, is dominated by structures with adsorbates on the bulk terminated surface blue colours. The right diagram is dominated by triangular reconstructions red and green colours. We note, that only the right diagram, constructed from DFT energy calculations with explicitly included solvation effects, is able to account for the experimental observation of triangular phases, as seen in in situ AFM experiments by Valtiner et al.

Stabilization of a conjugate base: solvation (video) | Khan Academy

To understand why triangular reconstructions are so strongly favoured by the electrolyte compared to the other considered surface reconstructions we evaluate the solvation energy, E solv. The solvation energy, which is the energy difference between the DFT total energy of the system in vacuum and the system in contact with the solvent, shows a dependence on both the amount of unpaired electrons at the surface Fig.

The strong selectivity towards non-metallic surface structures is a consequence of the screening propensity of the respective surfaces. Metallic surfaces, which have a much higher intrinsic electronic polarizability, can screen electrostatic charges much more efficiently compared to semiconducting surfaces. Consequently, the solvent provides an almost metallic screening the dielectric constant of water is 80 to surfaces, which are semiconducting, reducing electrostatic penalties at the surface.

For surfaces with metallic character i. Furthermore, surfaces experiencing a higher electrostatic penalty in vacuum naturally gain more energy by screening. Thus, triangular reconstructions, which are unfavourable from an electrostatic point of view in vacuum, due to the large separation between negative charges at the triangle edges filled O dangling bonds and positive charges inside the triangle empty Zn dangling bonds , will gain a higher solvation energy compared to the non-triangular structures.

The correlations identified in this study reveal that the solvation effects are substantial, highly discriminating and key to understand and eventually control the appearance and thermodynamic stability of structures at semiconducting surfaces.

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Valtiner, M. Todorova, G. Grundmeier, and J. Van de Walle and J. Freysoldt, B.

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Grabowski, T. Hickel, J.

Solvation, Lattice Energy and Hydration Energy

Neugebauer, G. Kresse, A. Janotti, and C. Van de Walle, First-principles calculations for point defects in solids, Rev. Todorova and J. Neugebauer, Extending the concept of defect chemistry from semiconductor physics to electrochemistry, Phys.


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