Fe- and Cu-oxides supported on γ-Al2O3 as catalysts for the selective catalytic reduction of NO with ethanol. Part I: catalyst preparation, characterization, and activity

Abstract

AbstractFe- and Cu-oxides supported on γ-alumina (γ-Al2O3; metal loading of 3 mass %) were investigated as alternative catalysts to the conventional Ag-based system in the selective catalytic reduction of NO with ethanol (EtOH-SCR). The catalysts were characterized by elemental analysis, N2 sorption, X-ray diffraction, temperature-prgrammed desorption of NH3, temperature-programmed reduction with H2, diffuse reflectance UV-VIS (DR-UV-VIS) spectroscopy, and compared with 3 mass % Ag/γ-Al2O3 as a reference catalyst. Catalytic experiments were carried out between 423 K and 773 K in the steady state and by temperature-programmed surface reaction (TPSR) experiments. For all catalysts, the highest NO conversion (900 ppm (ppm = parts of the mixture component per million parts of all mixture components) NO, 900 ppm EtOH, 0.5 vol. % H2O, 4 vol. % O2 in He) was found at 573 K. While 84 % of NO were converted over the Ag-based catalysts, only 20–60 % NO conversion was observed for the Fe- and Cu-containing catalysts. Total oxidation of ethanol as an unwanted side reaction occurs over 3 mass % Cu on γ-Al2O3 already at 573 K, whereas the highest activity of 3 mass % Fe on γ-Al2O3 for this conversion was reached at 743 K. For lower temperatures, partial oxidation of ethanol leads to organic by-products which can act as active intermediates in EtOH-SCR. TPSR experiments show that ethanol reacts over both the Fe- and the Cu-based catalysts to organic by-products, such as ethene or acetaldehyde, which affect the EtOH-SCR reaction.