Theoretical investigation of selective catalytic reduction of NO on MIL-100-Fe

文献情報

出版日 2017-12-20

DOI 10.1039/C7CP06756A

インパクトファクター 3.676

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要旨

MIL-100-Fe, a three-dimensional porous metal organic framework material, shows good activity for the selective catalytic reduction of NO by ammonia. Understanding reaction mechanisms at the molecular level contributes to the design and development of highly active catalysts. Herein, density functional theory calculations with the consideration of van der Waals interactions were performed to investigate the SCR mechanism on MIL-100-Fe. Lewis acid sites and Brønsted acid sites both exist on MIL-100-Fe, which are active for the SCR reaction. MIL-100-Fe exhibits the features of single-site catalysts, thus we calculated the NH3-SCR reaction process following the Eley–Rideal mechanism. The proposed NH3-SCR mechanism can be subdivided into two parts: (1) NO oxidation and (2) fast SCR reaction. Our results show that Lewis acid sites play an essential role in activating the reactants. The NO molecule is readily oxidized to NO2 species on the Fe Lewis acid sites, the adsorbed NH3 species react with gaseous NO2, and the formation of intermediate NH2NO is the rate-determining step. This study offers new and important insights into the mechanistic understanding of the NH3-SCR reaction on the MIL-100-Fe catalyst.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 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.