In this paper two different methods for the preparation of copper-containing catalysts have been described. Copper (II) ethylacetoacetate or copper (II) nitrate metallic precursors have been immobilized onto previously organofunctionalized MCM-41 material with N-4-(3-(triethoxysilyl)propyl)pyrimidine-2,4,6-triamine (DAPyPTS) compound. The amino hybrid materials have been prepared by using both post-synthesis and co-condensation methods. In addition, the immobilization has been performed using organic and aqueous media. The catalysts have been characterized using X-ray diffraction (XRD), N-2 adsorption-desorption, inductively coupled plasma-atomic emission spectroscopy (ICP-AES), scanning electron microscope (SEM) with energy-dispersive X-ray (EDX), elemental analysis, H-1, C-13 and Si-28 MAS NMR, FT-IR and DRUV-vis spectroscopy. Copper-containing catalysts have been tested in the benzyl alcohol oxidation with TBHP and H2O2 as oxidants and under solventless conditions. High selective (97%) to benzaldehyde was achieved using TBHP as oxidant and copper (II) ethylacetoacetate immobilized onto organofunctionalized MCM-41 as catalyst under solventless conditions. (C) 2011 Elsevier B.V. All rights reserved.