Journal of Molecular Catalysis A-Chemical, Vol.411, 279-289, 2016
Solvent-free oxidation of cyclohexane over covalently anchored transition-metal salicylaldimine complexes to alpha-zirconium phosphate using tert-butylhydroperoxide
Heterogeneous catalysts were prepared by covalent bonding of transition-metal salicylaldimine complex to alpha-zirconium phosphate, abbreviated as {alpha-ZrP.M(salicylaldimine) where M = Co, Mn and Cu}. The resulting compounds were characterized by BET surface area, TGA analysis, X-ray diffraction, Scanning electron micrograph, energy dispersive X-ray analysis, Fourier transform infrared and Atomic absorption spectroscopy. The catalytic activity of alpha-ZrP.M(salicylaldimine) was studied for the liquid phase oxidation of cyclohexane using terr-butylhydroperoxide as an oxidant under solvent free condition. In the oxidation reaction, cyclohexane was oxidized to cyclohexanol, cyclohexanone and some unidentified products. It was found that the reactivity of alpha-ZrP.M(salicylaldimine) catalyst for the oxidation reaction decreased in the order alpha-ZrP.Co(salicylaldimine) > alpha-ZrP.Mn(salicylaldimine) > alpha-ZrP.Cu(salicylaldimine). A maximum conversion of cyclohexane (14.18%) and selectivity of cyclohexanol (4.99%), cyclohexanone (87.34%) and some other products (7.67%) was observed for catalyst, alpha-ZrP.Co(salicylaldimine) after 6 h at 353 K. The catalyst, alpha-ZrP.Co(salicylaldimine) was reused for four cycles without significant loss of catalytic activity. (C) 2015 Elsevier B.V. All rights reserved.
Keywords:alpha-Zirconium phosphate;Salicylaldimine complex;tert-Butylhydroperoxide;Cyclohexane oxidation