RESUMO
Graphene oxide (GO) was synthesised via the oxidation of graphite and was characterised using ATR FTIR, PXRD, SEM, TEM and TGA. These techniques confirmed the presence of characteristic oxygen-containing functional groups and the resulting increase in interlayer spacing in the nanostructure. GO is used as the support to form nanocomposites composed of combinations of the following: iron oxide nanoparticles (Fe3O4), carbon nanotubes (CNT) and palladium nanoparticles (Pd). The four final nanocomposites formed are: Pd/GO, Pd/Fe3O4/GO, Pd/CNT/GO, and Pd/CNT/Fe3O4/GO. Key intermediates were analysed using ATR FTIR for the confirmation of the modification. Additionally, all composites and their precursors underwent electron microscopic analysis to visually assess composite morphologies and the size distribution of deposited nanoparticles. The Fe3O4 and Pd nanoparticles were indistinguishable from each other in their spherical shape and particle diameters, which were no bigger than 32 nm. From the TGA, incorporation of Fe3O4, CNT and finally Pd into the nanocomposites increased total thermal stability in terms of mass percentage lost over the temperature programme. GO showed significant decomposition, with all nanocomposites remaining relatively stable up to 120 °C. ICP OES results showed total Pd content by mass percentage for each final composite, varied from 7.9% to 9.1% mass Pd/collective mass. XPS confirmed the expected elemental compositions of composites according to their structures and the Pd0 : PdII ratios are obtained. The nanocomposites were tested for the catalytic reduction of nitrophenols. Pd/CNT/Fe3O4/GO gave the highest TOF' for the reduction of 4-NP and 2-NP. For the reduction of 3-NP, Pd/GO showed the highest TOF'. Nitrophenol's pK a and catalyst TOF' correlated in a direct proportional relationship for Pd/GO and Pd/Fe3O4/GO. It was found that Pd0 surpassed PdII in catalytic activity. Reduction of PdII to Pd0 took place during the first catalytic cycle.
