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Effect of the modification of ZrO2-containing pillared clay with Pt and Cu atoms on the properties of inorganic complex intermediates in the selective catalytic reduction of nitrogen oxides with propylene according to in situ IR-spectroscopic data

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Abstract

It was found that only bridging and bidentate nitrate complexes were formed on the surface of Pt,Cu/ZrO2-pillared interlayered clay (ZrO2-PILC) upon the interaction with a flow of the (0.2% NO + 2.5% O2)/N2 mixture, whereas monodentate and nitrosyl complexes were not detected. The concentration of nitrate complexes on Pt,CU/ZrO2-PILC was higher and the strength of their bond to the surface was weaker than those on unmodified ZrO2-PILC. Isopropoxide and acetate complexes and coordinatively bound acetone were formed on the surface in the interaction of Pt,Cu/ZrO2-PILC with a flow of the (0.2% C3H6 + 2.5% O2)/N2 mixture. The supporting of Pt and Cu onto zirconium dioxide pillars resulted in considerable changes in the concentration and the temperature region of the existence of hydrocarbon surface compounds, as compared with ZrO2-PILC. Under reaction conditions at relatively low temperatures, isopropoxide and nitrate intermediates on the surface of Pt,Cu/ZrO2-PILC formed a complex structurally similar to adsorbed dinitropropane. At elevated temperatures, a surface nitromethane complex was formed in the interaction of the acetate complex with nitrate species. The spectrokinetic measurements demonstrated that the apparent rate constants of consumption of nitrate and nitroorganic complexes considerably increased on going from ZrO2-PILC to Pt,Cu/ZrO2-PILC. Moreover, the constants of consumption of nitroorganic and nitrate complexes were similar for both of the catalysts. This fact suggests that, on the test catalysts, nitroorganic complexes were reaction intermediates in the selective catalytic reduction of NOx (NOx SCR) with hydrocarbons. The found differences in the activation species and thermal stabilities of reactants can explain different activities of ZrO2-PILC and Pt,Cu/ZrO2-PILC in the SCR reaction of NOx with propylene in an excess of oxygen.

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Authors and Affiliations

  1. Semenov Institute of Chemical Physics, Russian Academy of Sciences, Moscow, 117977, Russia

    V. A. Matyshak, K. A. Chernyshov, O. N. Sil’chenkova & V. N. Korchak

  2. Topchiev Institute of Petrochemical Synthesis, Russian Academy of Sciences, Moscow, 117912, Russia

    V. F. Tret’yakov & T. N. Burdeinaya

  3. Boreskov Institute of Catalysis, Siberian Branch, Russian Academy of Sciences, Novosibirsk, 630090, Russia

    V. A. Sadykov

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  1. V. A. Matyshak
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  2. V. F. Tret’yakov
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  3. T. N. Burdeinaya
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  5. V. A. Sadykov
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  6. O. N. Sil’chenkova
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Original Russian Text © V.A. Matyshak, V.F. Tret’yakov, T.N. Burdeinaya, K.A. Chernyshov, V.A. Sadykov, O.N. Sil’chenkova, V.N. Korchak, 2007, published in Kinetika i Kataliz, 2007, Vol. 48, No. 1, pp. 81–90.

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Matyshak, V.A., Tret’yakov, V.F., Burdeinaya, T.N. et al. Effect of the modification of ZrO2-containing pillared clay with Pt and Cu atoms on the properties of inorganic complex intermediates in the selective catalytic reduction of nitrogen oxides with propylene according to in situ IR-spectroscopic data. Kinet Catal 48, 74–83 (2007). https://doi.org/10.1134/S0023158407010119

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  • DOI: https://doi.org/10.1134/S0023158407010119

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