The role of hydroxylation in the step stability and in the interaction between steps: a first-principles study of vicinal MgO surfaces
文献信息
Fabio Finocchi, Pascale Geysermans, Antonin Bourgeois
Atomic structure and thermodynamic stability of vicinal MgO surfaces showing monoatomic steps are studied using density functional theory. We extend the general definition of step energy to the case of ledges that are covered by adsorbates. Using this definition, we consider the effect of hydroxylation on the thermodynamic stability of steps, either polar or non-polar, on (001) or (011) terraces. Clean non-polar steps along [100] on MgO(001) are the most stable ones. Upon water adsorption, the free energy of all hydroxylated ledges, almost independently of their orientation, is significantly reduced and approaches thermal energies for increasing water pressure, favoring the formation of hydroxylated steps on MgO surfaces. Furthermore, we show that interaction between polar steps can be either repulsive or attractive. This quite unusual behavior is described in terms of electrostatic interactions between ledges.
期刊推荐

Journal of Catalysis

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Pure and Applied Chemistry

Proceedings of the National Academy of Sciences of the United States of America

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Journal of Physics and Chemistry of Solids
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Physical Chemistry Chemical Physics

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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