• Gustavo P Romanelli

      Articles written in Journal of Chemical Sciences

    • Role of vanadium and pyridine in heteropolycompounds for selective oxidation of alcohols with hydrogen peroxide

      Valeria Palermo Paula I Villabrille Patricia G Vázquez Carmen V Cáceres Pietro Tundo Gustavo P Romanelli

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      This study describes the application of heteropolyacids H3PMo12O40,H4SiMo12O40, H4PMo11VO40, H5PMo10V2O40, H9PMo6V6O40, and a hybrid pyridine-modified heteropolyacid with Keggin structure for selective oxidation of alcohols to ketones or aldehydes using aqueous hydrogen peroxide and acetonitrile as solvent. Performance of these different catalysts in 1-phenylethanol oxidation was studied. Influence of reaction temperature, amount of catalyst and hydrogen peroxide and reaction time on the yield of acetophenone was investigated to obtain optimal reaction conditions. Oxidation ability of the catalyst depended on the number of vanadium atoms present in the Keggin ion and to a lesser extent on pyridine substitution in the Keggin secondary structure. In order to explore the applicability of the method for selective oxidation of alcohols to ketones or aldehydes, various alcohols were investigated according to the general procedure using hybrid pyridine-modified heteropolyacid.

    • Transition metal-modified polyoxometalates supported on carbon as catalyst in 2-(methylthio)-benzothiazole sulfoxidation

      Romina A Frenzel Gustavo P Romanelli Mirta N Blanco Luis R Piz

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      Polyoxometalates with lacunary Keggin structure modified with transition metal ions [PW11O39M(H2O)]5−, where M = Ni2+, Co2+, Cu2+ or Zn2+, were synthesized and supported on activated carbon to obtain the PW11MC catalysts. Using FT-IR and DTA-TGA it was concluded that the [PW11O39M(H2O)]5− species are interacting with the functional groups of the support, and that thermal treatment leads to the loss of the coordinatively bonded water molecules without any noticeable anion degradation. The activity and selectivity of the catalysts in the sulfoxidation reaction of 2-(methylthio)-benzothiazole, an emerging environmental pollutant, were evaluated. The reaction was carried out in acetonitrile as solvent using H2O2 35% p/v as a clean oxidant. The conversion values decreased in the following order: PW11NiC > PW11CuC > PW11CoC > PW11ZnC, with selectivity to sulfoxide higher than 69%. The catalyst could be reused without appreciable loss of the catalytic activity at least three times. The materials were found to be efficient and recyclable catalysts for 2-(methylthio)-benzothiazole sulfoxidation in order to obtain a more biodegradable product than the corresponding substrate.

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