A DFT+U study of the lattice oxygen reactivity toward direct CO oxidation on the CeO2(111) and (110) surfaces
文献信息
Fendy Chen, Di Liu, Jie Zhang, P. Hu, Xue-Qing Gong, Guanzhong Lu
Density functional theory calculations corrected by on-site Coulomb interaction have been carried out to track down the lattice oxygen reactivity of CeO2(111) and (110) surfaces in direct oxidation of a single CO. The possible elementary steps in CO adsorption and subsequent reactions with lattice oxygen were systematically studied. From calculated energetics, we determined that the lattice oxygen of the (110) surface is more reactive than that of the (111) surface. By calculating the reaction pathways leading to different final products, we found that the formation of carbonate species is competitive to CO2 formation and desorption, and such an effect could be more significant at CeO2(110) compared to CeO2(111). More importantly, it has also been found that electron localization at the characteristic 4f orbital of Ce, directly determined by subtle structural relaxation, can give rise to a unique scenario of the overall reaction coordinates. These results may bring us one step ahead toward the comprehensive understanding of catalytic performance of CeO2-based materials.
期刊推荐

Pure and Applied Chemistry

Science Progress

Planta Medica

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

Journal of Physics and Chemistry of Solids

Russian Chemical Reviews

Kinetics and Catalysis

Journal of Organometallic Chemistry

Science

Organic Preparations and Procedures International
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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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