Journal of Molecular Catalysis A-Chemical, Vol.381, 9-15, 2014
Deposition of fullerene C-60 on the surface of MCM-41 via the one-step wet impregnation method: Active catalysts for the singlet oxygen mediated photooxidation of alkenes
A series of C-60 catalysts supported on MCM-41 was prepared for the singlet oxygen-mediated oxidation of alkenes to the corresponding hydroperoxides (ene or Schenck reaction). The one-step wet impregnation method, followed by heating at 180 degrees C, was used for dispersing effectively 6, 9 and 12 wt% C-60 onto the MCM-41 surface. N-2 adsorption-desorption measurements, FT-IR. XRD, DRS and TGA were used to characterize the prepared photocatalysts. The photocatalytic activity of the C-60/MCM-41 series was determined by using the photooxygenation of 2-methyl-2-heptene as a probe reaction. The results of the present study were compared with those obtained in our previous studies where the same photocatalysts had been prepared by using the successive wetness impregnation method. It was found that very effective C-60/MCM-41 photocatalysts can be synthesized by applying the one-step wet impregnation method. All three photocatalysts exhibited similar activity in terms of substrate conversion, whereas their intrinsic activity which is expressed by the TON or TOF values, decreased with increasing C-60 content. The replacement of the successive incipient wetness impregnation by the simpler wet impregnation method provokes an increase in the photocatalytic activity of the samples with C-60 content equal to 9 and 12 wt% but it does not affect the photocatalytic activity of the sample with C-60 content equal to 6 wt%, which exhibits the maximum intrinsic activity. The influence of the deposition method and the C-60 loading on the photocatalytic performance of the C-60/MCM-41 catalysts was rationalized on the basis of the different size of the supported C-60 crystallites. (C) 2013 Elsevier B.V. All rights reserved.
Keywords:Photocatalysis;Singlet oxygen;Photooxidation;Supported C-60 catalysts;MCM-41;Ene or Schenck reaction