RODRIGO FERNANDO BRAMBILLA DE SOUZA

RODRIGO FERNANDO BRAMBILLA DE SOUZA

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PdxNiy/TiO2 Electrocatalysts for Converting Methane to Methanol in An Electrolytic Polymeric Reactor - Fuel Cell Type (PER-FC)
2023 - COELHO, JESSICA F.; GUTIERREZ, ISABELY M.; PEREIRA FILHO, NIVALDO G.; ZAMBIAZI, PRISCILLA J.; OLIVEIRA NETO, ALMIR; SOUZA, RODRIGO F.B. de
PdxNiy/TiO2 bimetallic electrocatalysts were used in fuel cell polymeric electrolyte reactors (PER-FC) to convert methane into methanol through the partial oxidation of methane promoted by the activation of water at room temperature. X-ray diffraction measurements showed the presence of Pd and Ni phases and TiO2 anatase phase. TEM images revealed mean particle sizes larger than those reported for PdNi materials supported, indicating that TiO2 promotes particle aggregation on its surface. Information on the surface structure of electrocatalysts obtained by Raman spectra indicated the presence or formation of NiO. The PER-FC tests showed the highest power density for the electrocatalyst with the lowest amount of nickel Pd80Ni20/TiO2 (0.58 mW cm􀀀2). The quantification of methanol through the eluents collected from the reactor showed higher concentrations of methanol produced, revealing that the use of TiO2 as a support also increased the reaction rate.
Desempenho eletrocatalítico de Pd/C e Pt/C para geração de energia a partir do extrato de cana-de-açúcar em célula a combustível de líquido direto
2023 - VILLARDI, BRUNO D.Q.; FILHO, NIVALDO G.P.; GOMES, PAULO V.R.; NANDENHA, JULIO; GODOI, CAMILA M.; TAGOMORI, THAIS L.; AZEREDO, NATHALIA; SOUZA, RODRIGO F.B. de; NETO, ALMIR O.; ZAMBIAZI, PRISCILLA J.
The processing of biomass to obtain fuels such as ethanol results in generating waste and polluting the environment. However, to meet energy demand and simultaneously reduce environmental pollution, fuel cells are promising devices for converting chemical compounds into electricity. Fuel cells can be powered by various types of liquids, including the sugars available in sugarcane extract, with high energy potential. Fuel cells employ the use of noble metals as electrocatalysts, such as Pt or Pd, to carry out the oxidation of these fuels. In this sense, this work reports the study of the oxidation of sugarcane extract in these different noble metals. The platinum catalyst was shown to be more active for the oxidation of sugars, resulting in a power density 10 times greater than Pd/C using a 50% diluted sugarcane extract solution, resulting in promising fuel cell systems. To produce ecologically correct electrical energy for the industry in general.
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.
PtSb/C electrocatalysts for glycerol oxidation in alkaline electrolyte
2022 - PEREIRA, C.V.; MAIA, V.A.; ZAMBIAZI, P.J.; SOUZA, R.F.B. de; ANTOLINI, E.; NETO, A.O.
Pt/C and PtSb/C catalysts in various atomic ratios were synthesized by the sodium borohydride reducing method and their activity for the glycerol oxidation reaction (GOR) was evaluated in alkaline media. Transmission Electron Microscopy (TEM) images showed that Pt particle size increases with increasing Sb content in the catalyst. X-ray photoelectron spectroscopy (XPS) showed that the ratio of Pt and Sb is close to that expected. By XPS measurements, the presence of Sb2O5 in Pt70Sb30/C and Pt50Sb50/C was observed. X-ray diffraction (XRD) analysis revealed the presence of the face-centered cubic (FCC) structure of Pt and PtSb and of some others phases that could be identified as Sb oxides. By linear sweep voltammetry (LSV) measurements, Pt80Sb20/C showed the highest activity for the GOR in alkaline media for potentials >−0.35 V vs. Ag/AgCl, while Pt50Sb50/C showed the highest GOR activity in the potential range between −0.60 and −0.35 V vs. Ag/AgCl. The direct glycerol fuel cells with Pt80Sb20/C as the anode catalyst showed the best performance. These results attest the beneficial effect of Sb addition to platinum: the activity enhancement in the presence of Sb atoms has to be ascribed to both a bifunctional mechanism related to the presence of Sb oxides, and an electronic effect between platinum and antimony in the PtSb alloy.
Electro-oxidation of ethanol in acid medium using carbon-supported PtRh nanoparticles with (100) preferential orientation
2021 - PEREIRA FILHO, N.G.; SOUZA, R.F.B.; RAMOS, A.S.; ANTONIASSI, R.M.; OLIVEIRA NETO, A.; SPINACE, E.V.
Carbon-supported PtRh nanoparticles with preferential (100) orientation was prepared by an alcohol-reduction process using KBr as a shape directing agent. The electrocatalysts were characterized by EDX (energy-dispersive X-ray analysis), XRD (X-ray diffraction) and TEM (Transmission electron microscopy). The electro-oxidation of ethanol was studied by cyclic voltammetry and chronoamperometry at room temperature in acid medium. On-line differential mass spectrometry experiments were performed on a single cell of a direct ethanol fuel cell (DEFC) at 60 0C and the anodic effluents were analyzed by ATR-FTIR. PtRh/C (100) electrocatalyst showed cubic-like morphology and average nanoparticles size of 8 nm and provided superior DEFC performance (density power per Pt active area) and CO2 selectivity compared to polycrystalline PtRh/C and commercial Pt/C electrocatalysts.
Glycerol dehydrogenation steps on Au/C surface in alkaline medium
2021 - FONTES, E.H.; RAMOS, C.E.D.; OTTONI, C.A.; SOUZA, R.F.B. de; ANTOLINI, E.; NETO, A.O.
The glycerol oxidation reaction (GLYOR) was evaluated using an Au/C electrocatalyst under alkaline conditions and varying glycerol (GLY) concentration. This electrocatalyst was synthesized by the borohydride reduction method. Au/C was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), and electrochemical techniques associated with in situ attenuated total reflectance Fourier transformed infrared spectroscopy (ATR-FTIR). XRD diffractograms showed the presence of Au (fcc). Cyclic voltammetry assisted by ATR-FTIR in situ measurements revealed that GLY oxidation on gold leads to the formation of a high amount of glyceraldehyde (GLYAD) for low GLY concentrations, while a lower amount of GLYAD was observed and the formation of dihydroxyacetone (DHA) was prevalent for high GLY concentrations. For high GLY concentrations DHA is almost stable, whereas for low GLY concentration DHA is fast oxidized to hydroxypyruvate. The excellent GLYOR activity of the Au/C catalyst in low GLY concentrations leads to the formation of deeper oxidized C1 species.
Methane conversion to higher value‑added product and energy co‑generation using anodes OF PdCu/C in a solid electrolyte reactor
2021 - GODOI, C.M.; SANTOS, M.C.L.; SILVA, A.J.; TAGOMORI, T.L.; RAMOS, A.S.; SOUZA, R.F.B. de; OLIVEIRA NETO, A.
PdxCuy/C catalysts combinations were employed to CH4 partial oxidation in mild condition using a solid electrolyte reactor—alkaline fuel cell type. The differential mass spectroscopy on line method was used to monitor the oxidation products obtained as methanol, dimethyl ether, methyl formate and potassium formate. It was observed that as the electrical potential of the reactor increases, the generation of products decreases. The best results for conversion of methane into methanol and energy co-generation was obtained from Pd90Cu10/ C and Pd50Cu50/ C due to better H2O activation effects and adsorption site for CH4 oxidation.
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.
Comparison of various atomic compositions of Au@Pd/C, Pd/C, and AuPd/C electrocatalysts for direct ethanol fuel cells
2020 - FONTES, ERIC H.; NANDENHA, JULIO; PIASENTIN, RICARDO M.; SOUZA, RODRIGO F.B. de; NETO, ALMIR O.
Pd/C, Au@Pd/C (core-shell), and AuPd/C (AR—consisting in Au microparticles) were used as electrocatalysts for ethanol oxidation in alkaline medium. A synergistic effect between Au and Pd atoms in Au@Pd/C makes the binding between ethanol and Au@Pd/C stronger. This leads to product formation in higher potentials and can be useful to select ethanol products. We also showed that the atomic composition of the electrocatalysts to be used in fuel cells and in powder form to be used in electrochemical experiments are very similar, reaching high values of correlation. The depth profiling X-ray photoelectron spectroscopy for the anode catalysts to be used in fuel cells can provide new insights about ethanol oxidation in direct ethanol fuel cells (DEFCs), for instance, metal oxide species can act in fuel cells environment. In terms of electric generation, Au@Pd/C presented a better performance in electrochemical experiments; the current density was about 1.6 times higher than the peak current density obtained for Pd/C. In terms of electrochemical stability, Au@Pd/C presented better final current density when compared to Pd/C and AuPd/C electrocatalysts. However, in DEFC experiments, Pd/C showed better performance.