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Development and Validation of a ReaxFF Reactive Force Field for Cu Cation/Water Interactions and Copper Metal/Metal Oxide/Metal Hydroxide Condensed Phases

2010; American Chemical Society; Volume: 114; Issue: 35 Linguagem: Inglês

10.1021/jp102272z

1520-5215

Adri C. T. van Duin, Vyacheslav S. Bryantsev, Mamadou S. Diallo, William A. Goddard, Obaidur Rahaman, Douglas J. Doren, David Raymand, Kersti Hermansson,

Analytical Chemistry and Sensors

To enable large-scale reactive dynamic simulations of copper oxide/water and copper ion/water interactions we have extended the ReaxFF reactive force field framework to Cu/O/H interactions. To this end, we employed a multistage force field development strategy, where the initial training set (containing metal/metal oxide/metal hydroxide condensed phase data and [Cu(H2O)n]2+ cluster structures and energies) is augmented by single-point quantum mechanices (QM) energies from [Cu(H2O)n]2+ clusters abstracted from a ReaxFF molecular dynamics simulation. This provides a convenient strategy to both enrich the training set and to validate the final force field. To further validate the force field description we performed molecular dynamics simulations on Cu2+/water systems. We found good agreement between our results and earlier experimental and QM-based molecular dynamics work for the average Cu/water coordination, Jahn−Teller distortion, and inversion in [Cu(H2O)6]2+ clusters and first- and second-shell O−Cu−O angular distributions, indicating that this force field gives a satisfactory description of the Cu-cation/water interactions. We believe that this force field provides a computationally convenient method for studying the solution and surface chemistry of metal cations and metal oxides and, as such, has applications for studying protein/metal cation complexes, pH-dependent crystal growth/dissolution, and surface catalysis.