THENNER SILVA RODRIGUES
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Artigo IPEN-doc 25099 Synthesis of highly dispersed gold nanoparticles on Al2O3, SiO2, and TiO2 for the solvent-free oxidation of benzyl alcohol under low metal loadings2019 - GUALTEROS, JESUS A.D.; GARCIA, MARCO A.S.; SILVA, ANDERSON G.M. da; RODRIGUES, THENNER S.; CANDIDO, EDUARDO G.; SILVA, FELIPE A. e; FONSECA, FABIO C.; QUIROZ, JHON; OLIVEIRA, DANIELA C. de; TORRESI, SUSANA I.C. de; MOURA, CARLA V.R. de; CAMARGO, PEDRO H.C.; MOURA, EDMILSON M. deWe reported the organic template-free synthesis of gold (Au) nanoparticles (NPs) supported on TiO2, SiO2, and Al2O3 displaying uniform Au sizes and high dispersions over the supports. The Au-based catalysts were prepared by a deposition– precipitation method using urea as the precipitating agent. In the next step, the solvent-free oxidation of benzyl alcohol was investigated as model reaction using only 0.08–0.05 mol% of Au loadings and oxygen (O2) as the oxidant. Very high catalytic performances (TOF up to 443,624 h-1) could be achieved. Specifically, we investigated their catalytic activities, selectivity, and stabilities as well as the role of metal–support interactions over the performances. The conversion of the substrate was found to be associated with the nature of the employed support as the Au NPs presented similar sizes in all materials. A sub-stoichiometric amount of base was sufficient for the catalyst activation and the observation of the catalysts profile over the time enable insights on their recyclability performances. We believe this reported method represents a facile approach for the synthesis of uniform Au-supported catalysts displaying high performances.Artigo IPEN-doc 24862 Marrying SPR excitation and metal–support interactions2018 - GEONMONOND, RAFAEL S.; QUIROZ, JHON; ROCHA, GUILHERME F.S.R.; OROPEZA, FREDDY E.; RANGEL, CLARA J.; RODRIGUES, THENNER S.; HOFMANN, JAN P.; HENSEN, EMIEL J.M.; ANDO, ROMULO A.; CAMARGO, PEDRO H.C.Plasmonic catalysis takes advantage of the surface plasmon resonance (SPR) excitation to drive or accelerate chemical transformations. In addition to the plasmonic component, the control over metal–support interactions in these catalysts is expected to strongly influence the performances. For example, CeO2 has been widely employed towards oxidation reactions due to its oxygen mobility and storage properties, which allow for the formation of Ce3+ sites and adsorbed oxygen species from metal–support interactions. It is anticipated that these species may be activated by the SPR excitation and contribute to the catalytic activity of the material. Thus, a clear understanding of the role played by the SPR-mediated activation of surface oxide species at the metal–support interface is needed in order to take advantage of this phenomenon. Herein, we describe and quantify the contribution from active surface oxide species at the metal–support interface (relative to O2 from air) to the activities in green SPR-mediated oxidation reactions. We employed CeO2 decorated with Au NPs (Au/CeO2) as a model plasmonic catalyst and the oxidation of p-aminothiophenol (PATP) and aniline as proof-of-concept transformations. We compared the results with SiO2 decorated with Au NPs (Au/SiO2), in which the formation of surface oxide species at the metal–support interface is not expected. We found that the SPR-mediated activation of surface oxide species at the metal–support interface in Au/CeO2 played a pivotal role in the detected activities, being even higher than the contribution coming from the activation of O2 from air.