Copper Containing Silicates as Catalysts for Liquid Phase Cyclohexane Oxidation

Copper containing silicates have been prepared by an acid-catalyzed sol-gel process. The materials were characterized by X-ray diffraction and fluorescence, EPR spectroscopy, elemental analysis, N2-physisorption, thermogravimetry, differential scanning calorimetry, temperature-programmed reduction, FTIR and UV/VIS spectroscopy. The silicates were shown to be efficient catalysts for the oxidation of cyclohexane with tert-butyl hydroperoxide as oxidant. Cyclohexanol and cyclohexanone were obtained as the main products. The metal was shown to be weakly bound to the silicate matrix and metal leaching was observed. Leaching was quantified by X-ray fluorescence and leaching tests showed that the catalytic activity is due to supported copper species. Leached copper showed no activity in the homogeneous phase.Silicatos contendo cobre foram preparados pelo processo sol-gel catalisado por ácido. Os materiais foram caracterizados por difração e fluorescência de raios X, espectroscopia EPR, análise elementar, fisissorção de N2, termogravimetria, calorimetria diferencial de varredura, redução à temperatura programada, espectroscopia FTIR e UV/VIS. Os silicatos mostram-se catalisadores eficientes para a oxidação do cicloexano com hidroperóxido de tert-butila como oxidante e obtiveram-se cicloexanona e cicloexanol como produtos principais da reação. O metal mostrou-se fracamente ligado à matriz de sílica e foi observada lixiviação do metal para a fase líquida. A lixiviação foi quantificada por fluorescência de raios X. Testes de lixiviação mostraram que a atividade catalítica é devida às espécies de cobre suportadas. O cobre lixiviado não mostrou nenhuma atividade catalítica em fase homogênea.170176Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq

Copper Containing Silicates as Catalysts for Liquid Phase Cyclohexane Oxidation

Copper containing silicates have been prepared by an acid-catalyzed sol-gel process. The materials were characterized by X-ray diffraction and fluorescence, EPR spectroscopy, elemental analysis, N2-physisorption, thermogravimetry, differential scanning calorimetry, temperature-programmed reduction, FTIR and UV/VIS spectroscopy. The silicates were shown to be efficient catalysts for the oxidation of cyclohexane with tert-butyl hydroperoxide as oxidant. Cyclohexanol and cyclohexanone were obtained as the main products. The metal was shown to be weakly bound to the silicate matrix and metal leaching was observed. Leaching was quantified by X-ray fluorescence and leaching tests showed that the catalytic activity is due to supported copper species. Leached copper showed no activity in the homogeneous phase