Gold nanoparticles have shown excellent activity for selective oxidation of alcohols; such catalytic systems are highly dependent on the initial activation of the substrates, which must occur on the catalyst surface in heterogeneous catalysts. In many cases, an extra base addition is required, although the basicity of the support may also be of significant importance. Here, we explored the intrinsic basicity of magnesium-based enrichments on CoFe2O4 magnetic nanoparticles for the oxidation of benzyl alcohol using molecular oxygen as oxidant. The MgO and Mg(OH)2 enrichments enabled gold impregnation, which was not possible on the bare CoFe2O4 nanoparticles. The Au/MgO/CoFe2O4 and Au/Mg(OH)2/CoFe2O4 catalysts reached 42% and 18% conversion, respectively without base promotion, in 2.5 hour and 2 bar of O2. When the catalysts were tested with sub-stoichiometric amounts of base, they became more active (>70% of conversion) and stable in successive recycling experiments without metal leaching, under the same reaction conditions. We also showed the oxide phases of the enrichments performed using Rietveld refinements and how the Mg(OH)2 phase interferes with the activity of MgO-based materials.
The development of stable and active gold catalysts has arisen as a significant strategy for oxidation of alcohols. Nano-size PVA-stabilized gold nanoparticles immobilized on Sr(OH)2 by colloidal deposition presented high catalytic activity for benzyl alcohol oxidation. In 2.5 h, 2 bar of O2 and without extra-base addition, the calcined support reached 54.6% (100 °C) and 67.4% (140 °C) of conversion, presenting the remarkable and unexplored intrinsic basicity that strontium-based materials retain. With sub-stoichiometric K2CO3 adding, under the same catalytic conditions, the catalyst conducted the reaction with similar activity, but with excellent reusability in the process, without any gold leaching. We investigated the influence that the support synthesis method and the solvent used for the NPs stabilization have on the oxidation activity. The produced materials were fully characterized by XPS, Rietveld refinement, and TEM.
1 January 2016 in Journal of the Brazilian Chemical Society
This work described a new magnetic material enriched with strontium as catalyst to produce babassu biodiesel. The use of magnetic materials has attracted attention due to easy and fast separation from reaction medium. Moreover, they are ecologically correct, due to they generate less discards to the environment. Techniques of analysis and characterization were carried out to check the synthesis of magnetite and strontium ferrite, besides to verify the presence of hydroxide and carbonate in the structure of the strontium oxide. The best catalytic activities presented conversions of 78.6% and 89.7% when using the catalysts SrO/Fe3O4 and SrO/SrFe2O4, respectively. Density studies of the alkali active sites were performed to elucidate the best activity for the catalyst composed with SrFe2O4.