Structure of clean and hydrated α-Al2O3 (102) surfaces: implication on surface charge

文献信息

发布日期 2011-03-07
DOI 10.1039/C0CP01295E
影响因子 3.676
作者

Sylvain Cristol


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摘要

Periodic DFT calculations coupled to a first-principle thermodynamic approach have allowed us to establish a surface phase diagram for the different terminations of the α-Al2O3 (102) surface in various temperature and water pressure conditions. Theoretical results are compared with previous experimental data from the literature. Under a wide range of temperature and water pressure (including ambient conditions) the most stable surface (denoted C2_1H2O in this work) is terminated with singly coordinated hydroxyls on four-fold coordinated aluminium (Al4C-μ1-OH) while most existing surface models are only considering six-fold coordinated surface Al atoms as in the bulk structure of alumina. The presence of more acidic Al4C-μ1-OH sites helps explain the low Point of Zero Charge (PZC) (between 5 and 6) determined from the onset of Mo oxoanions adsorption on (102) single crystal wafers. It is also postulated that another termination (corresponding to the hydration of the non-polar, stoichiometric surface, stable in dehydrated conditions) may be observed in aqueous solution depending on the surface preparation conditions.

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来源期刊

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
自引率: 10.3%
年发文量: 3036

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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