Molecular dynamics simulations of surface oxide–water interactions on Pt(111) and Pt/PtCo/Pt3Co(111)

Literature Information

Publication Date 2011-10-13
DOI 10.1039/C1CP22490E
Impact Factor 3.676
Authors

Rafael Callejas-Tovar


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Abstract

Classical molecular dynamics simulations of the interactions of water with oxidized Pt(111) and Pt/PtCo/Pt3Co(111) surfaces are performed by modeling water with the CF1 central force model that allows molecular dissociation and therefore the presence of other intermediates of the oxygen reduction reaction different from atomic oxygen. It is found that the water–surface oxide interactions do not affect the overall structure of the catalyst represented by an extended periodic slab. However, such interactions are affected by changes in the electrochemical potential which are simulated by higher values of the surface and atomic oxygen charges at increased oxygen coverage. Thus, electrochemical potential as well as the presence of protons and anions products of acid dissociation define the identity and the amount of oxygen reduction reaction intermediates such as OH or H3O. We observe agglomerations of water molecules over regions of the surface and the presence of OH and H3O in their vicinity. Our simulation model is able to qualitatively reproduce features of the degradation of the catalyst surface after oxidation and reduction cycles.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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