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An Atomistic Description of the γ-Alumina/Water Interface Revealed by Ab Initio Molecular Dynamics

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IFP Energies nouvelles, Direction Catalyse et Séparation, Rond-point de l’échangeur de Solaize, BP 3, 69360 Solaize, France
Physico-Chimie des Surfaces, PSL Research University, CNRS, Institut de Recherche de Chimie Paris, Chimie ParisTech, 11 rue Pierre et Marie Curie, 75005 Paris, France
Cite this: J. Phys. Chem. C 2017, 121, 19, 10351–10363
Publication Date (Web):April 19, 2017
Copyright © 2017 American Chemical Society

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    We report ab initio molecular dynamics (AIMD) simulations of the (100) and (110) γ-Al2O3/water interfaces at 300 K, using two sets of supercell models for each surface and two time lengths of simulation (10 and 40 ps). We first show that the effect of liquid water on the vibrational frequencies of hydroxyl groups at the interface varies according to the type of surface. This trend is explained by two key parameters affecting the interaction of both surfaces with water: the nature of the OH groups (i.e., μ1-OH, μ1-H2O, μ2-OH, and μ3-OH) and H-bond network among surface OH groups. The hydroxylated (110) surface favors the local structuration of water at the interface and the solvation of its μ1-OH and μ1-H2O groups by water similarly as in bulk liquid water. By contrast, on the (100) surface, a stronger H-bond network among μ1-OH and μ1-H2O groups reduces the water/surface interaction. We illustrate also how the interfacial interacting sites are spatially organized on the surfaces by two-dimensional maps of O–H distances. On both surfaces, the interfacial water layer orientation is predominantly Hup–Hdown. For long AIMD simulation time, Grotthuss-like mechanisms are identified on the (110) surface.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.7b00101.

    • (S1) Simulation cells used for the two larger models, (S2) radial distribution functions of liquid water, (S3) raw infrared spectra of the SLI before smoothing, (S4) complementary radial distribution functions calculated on the larger supercells, (S5) atomic relative concentrations at SLI for the smaller supercells, and (S6) radial distribution functions for the smaller supercells (PDF)

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