The role of low-coordinate oxygen on Co3O4(110) in catalyticCO oxidation

文献信息

发布日期 2010-11-09
DOI 10.1039/C0CP01138J
影响因子 3.676
作者

De-en Jiang


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摘要

A complete catalytic cycle for carbon monoxide (CO) oxidation to carbon dioxide (CO2) by molecular oxygen on the Co3O4(110) surface was obtained by density functional theory plus the on-site Coulomb repulsion (DFT + U). Previously observed high activity of Co3O4 to catalytically oxidize CO at very low temperatures is explained by a unique twofold-coordinate oxygen site on Co3O4(110). The CO molecule extracts this oxygen with a computed barrier of 27 kJ/mol. The extraction leads to CO2 formation and an oxygen vacancy on Co3O4(110). Then, the O2 molecule dissociates without a barrier between two neighboring oxygen vacancies (which are shown to have high surface mobility), thereby replenishing the twofold-coordinate oxygen sites on the surface and enabling the catalytic cycle. In contrast, extracting the threefold-coordinate oxygen site on Co3O4(110) has a higher barrier. Our work furnishes a molecular-level mechanism of Co3O4's catalytic power, which may help understand previous experimental results and oxidation catalysis by transition metal oxides.

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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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