RODRIGO FERNANDO BRAMBILLA DE SOUZA

RODRIGO FERNANDO BRAMBILLA DE SOUZA

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Conversion of nitrogen to ammonia using a Cu/C electrocatalyst in a polymeric electrolyte reactor
2023 - MAIA, VICTORIA A.; SANTOS, CAMILA M.G.; AZEREDO, NATHALIA F.B.; ZAMBIAZI, PRISCILLA J.; ANTOLINI, ERMETE; NETO, ALMIR O.; SOUZA, RODRIGO F.B. de
The electrochemical conversion of N2 to NH3 using a polymeric electrolyte reactor is a promising method to accelerate the green production of hydrogen carriers. On this basis, we report the efficiency of ammonia production by the nitrogen reduction reaction using a Cu/C catalyst in a polymeric electrolyte membrane reactor. The Cu/C catalyst was prepared by the NaBH4 reduction method and characterized by X-ray diffraction, transmission electron microscopy, cyclic voltammetry, and conversion experiments performed in a polymer electrolyte membrane fuel cell type reactor. The X-ray diffraction results showed the presence of CuO2 and carbon phases, while the TEM images showed a high agglomeration of copper nanoparticles on carbon. The onset potential of nitrogen reduction was near to the Cu (I) to Cu0 reduction peak. Mass spectroscopy was used to observe the production of N2H2 and NH3 and the consumption of N2. Maximum ammonia production was detected at 0.0 V with a NH3 yield rate of 38.4 µg h−1 cm−2 and a faradaic efficiency of 42.57 %.
Methane‑to‑methanol conversion and power co‑generation on palladium
2022 - COELHO, JESSICA F.; FILHO, NIVALDO G.P.; GUTIERREZ, ISABELY M.; GODOI, CAMILA M.; GOMES, PAULO V.R.; ZAMBIAZI, PRISCILLA J.; SOUZA, RODRIGO F.B. de; NETO, ALMIR O.
The use of palladium nickel catalysts with different compositions supported metal oxides, such as Sb2O5·SnO2 (ATO) catalyst combinations were employed to convert the methane-to-methanol in mild conditions using a fuel cell polymer electrolyte reactor. The catalysts used for the conversion of methane to methanol were characterized by XRD and observed the phases of ATO, the face-centered cubic structure of the Pd and Ni phases. All nanoparticles have a mean size between 9 and 12 nm as measured by TEM images. The products obtained from the methane oxidation, such as methanol and formate, were monitored using FT-IR spectroscopy to qualify the products formation, while High-Performance Liquid Chromatography was used to quantify them. In these studies, it was observed that as the electrical potential of the reactor increases, the generation of products decreases. The best results for the conversion of methane into methanol and energy co-generation were obtained from Pd50Ni50/ATO.
Silver nanoparticles-based hydrogels synthetized by ionizing radiation for cleaning of tangible cultural heritage surfaces
2022 - OLIVEIRA, MARIA J.A.; OTUBO, LARISSA; PIRES, ADRIANA; BRAMBILLA , RODRIGO F.; CARVALHO, ANA C.; SANTOS, PAULO S.; OLIVEIRA NETO, ALMIR; VASQUEZ, PABLO
The surfaces of the works of art are one of their most important parts since they interact directly with the observer's perception. On the other hand, they are also in direct contact with physical, chemical and biological agents that can induce degradation and signs of aging. Dust deposits, stains and aged layers of protection can degrade, causing irreversible damage to works of art. In this way, the removal of undesirable materials from artistic surfaces is essential to preserve cultural heritage articles. The aim of this work was to develop silver nanoparticles-based hydrogels and to study the behavior regarding solvent concentration, stability and ability to clean dirt samples based on paper and canvas. The hydrogels were synthesized (reticulated) by gamma rays having the simultaneous formation of silver nanoparticles (AgNP) in the same process. The samples were characterized by swelling tests, attenuated total reflection Fourier-transform infrared spectroscopy (ATR-FTIR), Raman spectroscopy, differential scanning calorimetry (DSC), transmission electron microscopy (TEM), scanning electron microscopy (SEM) and optical microscopy (OM). The results showed the removal of dirt from the paper samples, as well as the softening of the dirt from the canvas, without leaving residues and without affecting the integrity of the art works submitted to treatment.
Methanol electrosynthesis from CO2 reduction reaction in polymer electrolyte reactors - fuel cell type using [6,6′-(2,2′-bipyridine-6,6′-diyl)bis(1,3,5-triazine-2,4-diamine)] (dinitrate-O) copper (II) complex
2022 - GARCIA, L.M.S.; FILHO, N.G.P.; CHAIR, K.; KAUR, P.; RAMOS, A.S.; ZAMBIAZI, P.J.; SOUZA, R.F.B. de; OTUBO, L.; DUONG, A.; NETO, A.O.
Electrocatalytic carbon dioxide reduction reaction has been an attractive way to convert greenhouse gas into valuable chemical fuels based on carbon-neutral energy. Therefore, it serves as an effective approach to combating high concentrations of CO2 in the atmosphere as well as reducing the use of fossil fuels responsible for emitting carbon dioxide and other greenhouse gases, meeting growing energy demands. In this work, the copper(II) bis-triazine bipyridine complex supported on carbon black has been applied as a catalyst in a polymeric electrolytic reactor – fuel cell type for converting CO2 into methanol. The physical and nanostructure properties of the Cu(II) nanocomposite were previously determined by Fourier transform infrared, Raman spectroscopy, X-ray powder diffraction, and transmission electron microscopy techniques. The electrocatalytic activity of the Cu complex catalyst was monitory by differential mass spectroscopy. The results indicate that the catalyst is not selective for the preferential synthesis of a specific product, but a mixture of products (methanol, formic acid, formaldehyde, carbon monoxide, and methane) was detected. According to our results, 2.5% and 5% Cu complex on carbon black were the ideal amounts for polymeric electrolytic reactor – fuel cell type applications to produce methanol from CO2 with faradaic efficiency of ∼22% for both compositions.
cis-[6-(pyridin-2-yl)-1,3,5-triazine-2,4-diamine](dichloride) palladium(II)-based electrolyte membrane reactors for partial oxidation methane to methanol
2022 - GARCIA, LUIS M.S.; ZAMBIAZI, PRISCILLA J.; CHAIR, KHAOULA; DOAN, TUAN D.; RAMOS, ANDREZZA S.; NANDENHA, JULIO; SOUZA, RODRIGO F.B. de; OTUBO, LARISSA; DUONG, ADAM; NETO, ALMIR O.
Methane is an abundant resource and the main constituent of natural gas. It can be converted into higher value-added products and as a subproduct of electricity co-generation. The application of polymer electrolyte reactors for the partial oxidation of methane to methanol to co-generate power and chemical products is a topic of great interest for gas and petroleum industries, especially with the use of materials with a lower amount of metals, such as palladium complex. In this study, we investigate the ideal relationship between cis-[6-(pyridin-2-yl)-1,3,5-triazine-2,4-diamine(dichloride)palladium(II)] (Pd-complex) nanostructure and carbon to obtain a stable, conductive, and functional reagent diffusion electrode. The physical and structural properties of the material were analyzed by Fourier transform infrared (FT-IR) and Raman spectroscopies, transmission electron microscopy (TEM), and X-ray powder diffraction (XRD) techniques. The electrocatalytic activity studies revealed that the most active proportion was 20% of Pd-complex supported on carbon (m/m), which was measured with lower values of open-circuit and power density but with higher efficiency in methanol production with reaction rates of r = 4.2 mol L–1·h–1 at 0.05 V.
CO2 reduction on Cu/C used as a cathode in a polymeric electrolyte reactor
2022 - LIMA, MARIANA; GODOI, CAMILA M.; SANTOS, MONIQUE C.L.; NANDENHA, JULIO; NETO, ALMIR O.; SOUZA, RODRIGO F.B. de
CO2 is one of the leading greenhouse gases, so studies that turn this gas into higher value-added products, that function as simpler and cheaper hydrogen stores, as an alcohols, are extremely important. In this work we using a polymeric Electrolyte Reactor– fuel cell type supplied with H2 on platinum anode and dry CO2 in the cathode with a copper-carbon electrocatalyst. Copper nanoparticles supported on carbon Vulcan XC72 were produced by the sodium borohydride reduction method. The XRD revealed the presence of two different phases, CuO and Cu2O. In addition, the TEM images revealed agglomerates presence. The water, formaldehyde, methanol, methane, formic acid, dimethyl ether, oxalic acid, dimethyl carbonate, and ethylene-glycol were observed by differential mass spectroscopy on line with the reaction and the onset potential for each product and these results were confirmed by infrared spectroscopy – ATR-FTIR setup. This work showed the mapping CO2 reduced compounds for onset potential proposing some contributions to the literature.
Partial methane oxidation in fuel cell-type reactors for co-generation of energy and chemicals
2022 - SOUZA, RODRIGO F.B. de; FLORIO, DANIEL Z.; ANTOLINI, ERMETE; NETO, ALMIR O.
The conversion of methane into chemicals is of interest to achieve a decarbonized future. Fuel cells are electrochemical devices commonly used to obtain electrical energy but can be utilized either for chemicals’ production or both energy and chemicals cogeneration. In this work, the partial oxidation of methane in fuel cells for electricity generation and valuable chemicals production at the same time is reviewed. For this purpose, we compile different types of methane-fed fuel cells, both low- and high-temperature fuel cells. Despite the fact that few studies have been conducted on this subject, promising results are driving the development of fuel cells that use methane as a fuel source for the cogeneration of power and valuable chemicals.
High CO tolerance of Pt nanoparticles synthesized by sodium borohydride in a time-domain NMR spectrometer
2020 - RAMOS, A.S.; SANTOS, M.C.L.; GODOI, C.M.; QUEIROZ, L.C. de; NANDENHA, J.; FONTES, E.H.; BRITO, W.R.; MACHADO, M.B.; NETO, A.O.; SOUZA, R.F.B. de
The CO poisoning effect was overcome using a novel synthesis method. This method consists of using sodium borohydride reducing agent assisted by magnetic field and radiofrequency pulses in the time-domain NMR spectrometer. This synthesis was useful to disperse the Pt nanoparticles over the carbon support and to compress the lattice strain of the Pt crystalline structure. Besides that, Pt/C MFP90° showed a multi-CO oxidation component in cyclic voltammetry, and this can avoid the poisoning effect by creating a large availability of CO species to be adsorbed, desorbed, and re-adsorbed. Pt/C MFP90° has also shown the best performance in the PEMFC regarding H2 and CO + H2 experiments.
Obtaining C2 and C3 products from methane using Pd/C as anode in a solid fuel cell-type electrolyte reactor
2020 - RAMOS, ANDREZZA S.; SANTOS, MONIQUE C.L.; GODOI, CAMILA M.; OLIVEIRA NETO, ALMIR; SOUZA, RODRIGO F.B. de
Methane was converted into C2 and C3 products under mild conditions using a single stage solid electrolyte reactor, using a proton exchange membrane fuel cell as a SER-FC and Pd/C as an electrocatalyst prepared by the reduction method of sodium borohydride. This electrocatalyst has a cubic pattern of palladium centered on the face and an average size of nanoparticles close to 6.4 nm, according to the literature. Differential mass spectrometry reveals the chemical profile of species obtained from the oxidation of methane with ionic currents (Ii) at m/z=16, 28, 30, 32, 44, 46 and 60. In many cases, Ii can be assigned to more than one species; therefore, complementary ATR-FTIR experiments were performed. The ATR-FTIR spectra confirmed the presence of C2 and C3 compounds such as ethane, ethanol, acetaldehyde, acetic acid and propane. Considering the low amount of water in the reaction medium, these results may be associated with the use of Pd/C electrocatalysts responsible for the activation of the water molecule.
Conversion of methane into methanol using the [6,6′-(2,2′-bipyridine-6,6′-diyl)bis(1,3,5-triazine-2,4-diamine)](nitrato-O)copper(II) complex in a solid electrolyte reactor fuel cell type
2020 - GARCIA, LUIS M.S.; RAJAK, SANIL; CHAIR, KHAOULA; GODOY, CAMILA M.; SILVA, ARACELI J.; GOMES, PAULO V.R.; SANCHES, EDGAR A.; RAMOS, ANDREZZA S.; SOUZA, RODRIGO F.B. de; DUONG, ADAM; NETO, ALMIR O.
The application of solid electrolyte reactors for methane oxidation to co-generation of power and chemicals could be interesting, mainly with the use of materials that could come from renewable sources and abundant metals, such as the [6,6′- (2, 2′-bipyridine-6, 6′-diyl)bis (1,3,5- triazine-2, 4-diamine)](nitrate-O)copper (II) complex. In this study, we investigated the optimal ratio between this complex and carbon to obtain a stable, conductive, and functional reagent diffusion electrode. The most active Cu-complex compositions were 2.5 and 5% carbon, which were measured with higher values of open circuit and electric current, in addition to the higher methanol production with reaction rates of 1.85 mol L−1 h−1 close to the short circuit potential and 1.65 mol L−1 h−1 close to the open circuit potential, respectively. This activity was attributed to the ability of these compositions to activate water due to better distribution of the Cu complex in the carbon matrix as observed in the rotating ring disk electrode experiments.