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Item Methanol tolerant electrocatalysts for the oxygen reduction reaction(Springer, 2015) Asteazaran, Mariano; Bengio, Silvina; Triaca, Walter; Castro Luna, AnaDirect methanol fuel cells (DMFCs) represent an interesting alternative in obtaining electricity in a clean and efficient way. Portable power sources are one of the most promising applications of passive DMFCs. One of the requirements in these devices is to use high alcohol concentration, which due to methanol crossover causes a considerable loss of fuel cell efficiency. In order to develop methanol tolerant cathodes with suitable activity, different supported catalysts namely PtCo/C and PtCoRu/C, were prepared either via ethylene glycol reduction (EG) with or without microwave heating assistance (MW) or via the alloy method, the latter followed by a thermal treatment in a reducing atmosphere (N2/H2). All cathode-catalysts were tested to determine the role of the components in simultaneously enhancing the oxygen reduction reaction (ORR) and discouraging the methanol oxidation reaction. According to the synthesis methodology, X-ray photoelectron spectra showed that the amount of metal oxides on the surface varies, being higher on the PtCo/C EG and PtCoRu/C EG catalysts. The electrochemical characterization of the catalysts was accomplished in a three electrodes electrochemical cell with a glassy carbon rotating disk electrode covered with a thin catalytic film as working electrode. To study the ORR and the influence of different methanol concentrations, linear sweep voltammetry and cyclic voltammetry were employed. The PtCo/C EG, with an important metal oxide amount on the surface, and the PtCoRu/C MW and EG electrodes, both with RuO2 on their surfaces, were the most tolerant to methanol presence.Item Preparation and evaluation of carbon supported catalysts for ethanol oxidation(Springer, 2013) Bonesi, Alejandro; Asteazaran, Mariano; Moreno, Mario; Bengio, Silvina; Zampieri, Guillermo; Triaca, Walter; Castro Luna, AnaSupported PtSnIr/C, PtSn/C, and IrSn/C catalysts with potential application in a direct alcohol fuel cell were prepared by chemical reduction employing Pechini methodology. The catalyst particles were characterized by high-resolution transmission electron microscopy, energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy (XPS). Linear sweep voltammetry (LV), chronoamperometry, and electrochemical impedance spectroscopy (EIS) measurements were performed by using a glassy carbon working electrode covered with the catalyst in a 1 M ethanol+0.5 M H2SO4 solution at 60 °C. It was demonstrated through XPS that PtSnIr/C and IrSn/C contain both IrO2 and SnO2. LV and chronoamperometry show a better catalytic behavior for ethanol oxidation on PtSnIr/C in the low-potential region and the improvement is attributed to the presence of both Sn and Ir oxides. The EIS accurately established that PtSnIr/C improved ethanol oxidation at lower potentials than PtSn/C.Item Síntesis de nano catalizadores para celdas de combustible de metanol directo(Revista Tecnología y Ciencia UTN, 2014) Asteazaran, Mariano; Bonesi, Alejandro; Triaca, Walter; Castro Luna, AnaLas celdas de combustible de metano/ directo, DMFCs, permiten una conversión completa de la energía de la reacción química (CH)3OH(ac)+3/2 O2(g)=7CO2(g)+2H2O(l) en energía eléctrica. El platino es el catalizador más utilizado en las DMFCs. Para poder generar cantidades aceptables de corriente no se puede prescindir del uso de este metal como catalizador. Como la catálisis se manifiesta a nivel superficial, si se sintetizan nano partículas catalíticas soportadas sobre negro de carbón se obtendrá una gran área de reacción. El empleo de la nano tecnología y la combinación de Pt con otros metales aumenta la actividad electro catalítica y reduce el costo de las celdas de combustible. Se sintetizan y se determinan las actividades electro catalíticas de nano partículas en base platino como material de electrodo para el cátodo donde se lleva a cabo la reacción de reducción de oxígeno en la DMFC.Item Research on methanol tolerant catalysts for the oxygen reduction reaction(Springer, 2015) Asteazaran, Mariano; Cespedes, German; Bengio, Silvina; Moreno, Mario; Triaca, Walter; Castro Luna, AnaDirect methanol fuel cells (DMFCs) generate electricity in a clean and efficient way, so they are a valuable alternative to traditional environmentally harmful technologies. Portable power sources are one of the applications of passive DMFCs. One of the requirements in these devices is the use of high alcohol concentration. Methanol permeation across the polymer electrolyte membrane (methanol crossover) causes a loss of fuel cell efficiency as the oxygen reduction reaction (ORR) and the methanol oxidation reaction (MOR) occur simultaneously at the cathode. To develop methanol-tolerant catalysts with suitable activity, different PtM/C and PtMRu/C combinations with M = Co or Fe were prepared by a modified impregnation method. The synthesized catalysts were studied to determine the role of the components in enhancing the ORR and simultaneously discouraging the MOR. The materials were characterized by TEM, XPS and EDS. Well-distributed particles for all the catalysts were shown by TEM. XPS spectra revealed that the method produces a great amount of metallic Pt. The electrochemical characterization was carried out by linear sweep voltammetry and cyclic voltammetry, in a three-electrode electrochemical cell with a glassy carbon rotating disk electrode covered with a thin catalytic layer and a Nafion film as the working electrode. Binary and ternary catalysts have a good activity for the ORR. However, the enhanced activity of binary catalysts is lost when the ORR is studied in the presence of methanol. Ternary catalysts containing Ru showed higher methanol-tolerance, regardless of the composition.Item Efectos de la membrana de intercambio de protones en el desempeño de una celda de combustible H2 O2(Revista Tecnología y Ciencia UTN, 2016) Cespedes, German; Castro Luna, AnaUna celda de combustible convierte directamente la energía química de un combustible en electricidad. Su desempeño depende de diferentes parámetros tales como el espesor de la membrana intercambiadora de protones, el contenido de humedad y la temperatura de la celda. Para realizar un estudio sistemático sobre como la variación de estos parámetros afectan la performance de la celda se propone un modelo matemático de poro simple y se aplica en la simulación de las curvas experimentales que muestran la variación del potencial de la celda cuando se drena corriente. Se observa que la variación del contenido de humedad y el espesor de la membrana intercambiadora de protones tienen un efecto tan pronunciado sobre la curva de polarización a diferencia de la temperatura de funcionamiento de la celda.Item Searching for suitable catalysts for a passive direct methanol fuel cell cathode(Elsevier, 2015) Asteazaran, Mariano; Cespedes, German; Moreno, Mario; Bengio, Silvina; Castro Luna, AnaTrimetallic PtMRu/C cathode catalysts with M ¼ Co or Fe obtained by an impregnation procedure using ethylene glycol and NaBH4 as reducing agent, with suitable activity for the oxygen reduction reaction (ORR) and improved tolerance to methanol, have been physically characterized by HRTEM, EDS and XPS. The examined nanoparticles have a small particle size and are well spread on the carbon support. Pt is mainly found as Pt(0) and Co, Fe and Ru are mostly oxidized. To study their durability and performance for ORR and methanol tolerance over time, the catalysts were subjected to an electrochemical accelerated stress test (AST), consisting in cycling the potential 2000 times. Polarization curves for ORR with and without methanol were recorded. After the AST the trimetallic PtMRu/C catalysts are able to keep their performance for ORR in the presence of methanol.Item Effect of water content in the gas diffusion layer of H2 O2 PEM fuel cell(Journal of Materials Science and Engineering, 2016) Cespedes, German; Asteazaran, Mariano; Castro Luna, AnaThe heart of a fuel cell is the membrane-electrode assembly consisting of two porous electrodes, where the electrochemical reactions take place, and the ionomer conductive membrane, which allows the proton exchange from the anode to the cathode. The porosity of the electrodes plays an important role in the fuel cell performance. One of the drawbacks presented by the porous electrodes is the accumulation of water in their structure, which implies a hindrance for the reactive gas transport to reach the catalytic reactive sites. In this paper, a mathematical model of a porous electrode, assuming single pores with uniform distribution, is introduced to determine the influence of water accumulation in the electrode on the fuel cell performance under different operating conditions. It is demonstrated that at low current densities, water accumulation has no effect in the fuel cell behavior, whereas at high current densities its performance is severely affected.