Density Functional Theory Molecular Cluster Study of Copper Interaction with Nitric Oxide Dimer in Cu−ZSM-5 Catalysts
| Autor: | Ivan I. Zakharov, Zinfer R. Ismagilov, Svetlana A. Yashnik, Olga I. Zakharova, Sergey Ph. Ruzankin, Vladimir F. Anufrienko |
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| Rok vydání: | 2007 |
| Předmět: |
biology
Dimer chemistry.chemical_element Active site Electron donor Electronic structure Photochemistry Copper Surfaces Coatings and Films Electronic Optical and Magnetic Materials Catalysis chemistry.chemical_compound General Energy chemistry biology.protein Physical chemistry Density functional theory Physical and Theoretical Chemistry ZSM-5 |
| Zdroj: | The Journal of Physical Chemistry C. 111:3080-3089 |
| ISSN: | 1932-7455 1932-7447 |
| DOI: | 10.1021/jp0650634 |
| Popis: | The various quantum chemical models of catalytic active site in Cu−ZSM-5 zeolites are analyzed. The density functional theory (DFT) is used to calculate the electronic structure of molecular cluster (HO)3Al−O−Cu−O−Cu modeling the catalytic active site in Cu−ZSM-5 zeolites and study the interaction and decomposition of NO. It is assumed that the rate-determining stage of the low-temperature selective catalytic reduction of NO is the formation of the π-radical (N2O2)- on electron donor sites of Cu−ZSM-5 catalysts. This is in good agreement with the high electron affinity of the molecular dimer ONNO (Ea = −1.5 eV) and is confirmed by the experimental data on the formation of surface anion π-radical (N2O2)- on electron donor sites of supported organo−zirconium surface complex. The DFT calculated electronic structure and excitation energy spectra for the model system (HO)3Al−O−Cu−O−Cu show that it is a satisfactory model for description of experimental UV−vis spectra of Cu−ZSM-5, containing (−O−Cu−O−Cu−) chain... |
| Databáze: | OpenAIRE |
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