Oxidação parcial de metano a compostos oxigenados (HCHO e CH3OH) sobre catalizadores oxidos MoOx/MgO-SiO2 e VOx-SiO2

AUTOR(ES)
DATA DE PUBLICAÇÃO

2003

RESUMO

Methane is the major component of natural gas, often present as more than 90% of the gas. Current1y it is primarily used as a fuel. In the chemical industry it is used in the production of synthesis gas, hydrogen, and in the manufacture of the halogen derivatives of methane, acetylene, hydrogen cyanide, technical carbon, and many other products. The direct conversion of methane to formaldehyde and methanol in a single catalytic step in sufficient1y high yield would give rise to new opportunities in the conversion of natural gas to other useful fuels and chemicals. Both the homogeneous and heterogeneous processes have been studied under various conditions although progress toward obtaining a yield that would make such a process industrially viable has been very slow. The majority of these studies have involved metal oxide catalysts. In this work, the selective oxidation of methane to oxygenated compounds (HCHO e CH3OH) at atmospheric pressure was studied on MoOxfMgO-SiO2 and VOx/MgO-SiO2. The mixed oxides of magnesia and silica were prepared in different atom ratios (Mg:Si = 1:0, 3:1,2:1, 1:1, 1:3, 1:2 or 0:1), dried at 400 K for 12 h and calcined at 1050 K for 5 h. The active phase, Mo (H24Mo7N6O24) or V (H4NO3 V), was added to the supports by the incipient wetness method. The percentages of Mo or V added to the mixed oxides were 0,1%, 1,67%,2,2%,3,25%,4,82% or 6,4%. The solids were characterized by X-ray diffraction, BET surface area and oxygen chemisorption. The objective of the present work was to study the influence of the introduction of MgO in the supports, of the amount of Mo and V on the surface of the supports and of the CH4:O2 molar ratios. Both supported Mo and V oxides were active in the conversion of methane to C1-oxygenates and Cox. The main products of the oxidation reaction were HCHO, CO and CO2. The partial oxidation products (HCHO, CH30H) were favored by high CH4:O2 molar ratios and formaldehyde was the first oxidation product, which was further oxidized to CO. The vanadium oxide catalysts were more active than the molybdenum oxide catalysts in conversion of methane. However, the higher reaction rate also resulted in a further oxidation of HCHO to CO

ASSUNTO(S)

molibdenio vanadio oxidação gas natural metanol catalizadores formaldeido metano

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