Browsing by Author "Ledesma , Brenda Cecilia"
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Item Experimental Desing Optimization of the tetralin Hydrogenation over Pt-Ir/SBA-15.(Univesidsad Tecnológica Nacional, 2015) Vallés , Verónica Alejandra; Ledesma , Brenda Cecilia; Rivoira , Lorena Paola; Cussa , jorgelina; Anunziata , Oscar Alfredo; Beltramone, Andrea Raquel; Anunziata , Oscar Alfredo; Cussa , jorgelina; Rivoira , Lorena Paola; Ledesma , BrendaThe oil refining industry has a difficult challenge to meet the increasingly stringent regula tions on environmental issues. Contaminants such as sulfur, nitrogen, fused ring aromatic compounds or metals are the principal to remove to achieve "green" fuels. The hydrotreating (HDT) is one of the processes most used in the refinery to remove these contaminants. To optimize the gas oil hydrotreater, it is crucial to understand the aromatic hydrogenation reac tion chemistry occurring in the gas oil hydrotreater. To find alternative processes, it is neces sary to develop new and more active catalysts to replace the current ones. Bimetallic Pt–Pd catalysts have received considerable attention, because they show high actvity in a variety of catalytic applications [1,2]. From a fundamental point of view, exploring bimetallic catalysts also allows better understanding of mechanisms and variables involved in the catalytic reac tions. The features of the catalysts here studied are going to be correlated with their catalytic performance in the hydrogenation of tetralin. The final goal is to find the optimal proportion of each metal in order to be more active and the best reaction conditions. The statistical expe riments design is the process of planning an experiment to obtain appropriate data that can be analyzed by statistical methods, to produce concrete and valid conclusions [3]. One of the main advantages in the response curve is to visualize the response for all levels of the experi mental factors Experiment design response surface methodology (RSM) is used in this work to model and to optimize the processItem Ir-Pt/SBA-15 applied in the optimization of tetralin hydrogenation.(Univesidsad Tecnológica Nacional, 2015) Vallés , Verónica Alejandra; Ledesma , Brenda Cecilia; Rivoira, Lorena Paola; Cussa , jorgelina; Anunziata , Oscar Alfredo; Beltramone, Andrea Raquel; Cussa , jorgelina; Ledesma , BrendaBimetallic catalysts have received considerable attention for hydrotreating (HDT) because they show high activity. The features of the catalysts here studied are going to be correlated with their catalytic performance in the hydrogenation of tetralin at mild conditions. The final goal is to find the optimal proportion of each metal in order to be more active and the best reaction conditions (temperature and amount of catalyst). The statistical experiments design is the process of planning an experiment to obtain appropriate data that can be analyzed by statistical methods, to produce concrete and valid conclusions. One of the main advantages in the response curve is to visualize the response for all levels of the experimental factors Experiment design response surface methodology (RSM) is used in this work to model and to optimize the process. Platinum and Iridium nanoparticles were incorporated into SBA-15 support by the wet co-impregnation method. Ir content was set as 1wt. % and Pt was varied from 0 to 1wt. %. The catalysts were characterized by XRD, BET, XPS, TEM, ICP and TPR. XRD profiles are characteristic of the two-dimensional p6mm hexagonal mesostructure with d100 spacing of 10.16 nm; where the d100 spacing upon Ir and Pt incorporation were quite similar to pristine SBA-15. The TEM images and XPS demonstrate that the metal particles were mainly present inside the porous and XPS and TPR corroborated the reduced state of the metals. The catalytic activity was measured in a 4563Parr reactor at 15 atm of hydrogen and 360 rpm. Feed consisted in 50 mL of tetralin in Dodecane, the amount of tetralin is set according to the ratio of catalyst mass/mass reagent corresponding to each reaction. The application of this methodology allows a better understanding of the influence of the different factors: content of metal on catalyst (A), relationship: mass of catalyst/reagent mass (B) and reaction temperature (C), on two responses: conversion at 3 h and at 5 h of reaction time. These factors were carefully selected taking account the influence of the parameters in the reaction. The design was analyzed by Statgraphics and Statistica Soft. We found that, the variable Catalyst has the best influence over the Conversion at the 95.0% confidence level, according to the Pareto.Item Novel and simple one-pot method for the synthesis of titanium modified-CMK-3 applied in desulfurization of refractory oeganosulfur compounds.(Univesidsad Tecnológica Nacional., 2018) Rivoira , Lorena Paola; Ledesma , Brenda Cecilia; Juárez , Juliana María; Beltramone, Andrea Rauqel; Juárez , Juliana María; Ledesma , Brenda CeciliaTi-CMK-3 carbon mesoporous was prepared using a novel synthesis method. This new method avoids the hard template synthesis used commonly. The method developed here, allows reducing time, energy consumption and cost. Our primary aim in this work is to evaluate the ODS activity of the Ti-modified mesoporous carbon CMK-3, synthesized by the short time method, in order to achieve total removal of sulfur compounds from diesel fuel. The catalytic oxidation of the sulfur compound with hydrogen peroxide was carried out in a glass batch reactor, equipped with a magnetic stirrer, a thermometer and a condenser. In a typical run, the solid catalyst (60 mg) was suspended under stirring (750 rpm) in 20 mL of a solution of 500 ppm of S as DBT (or other) in acetonitrile. Then, appropriate amount of 30% aqueous H2O2 was added at constant temperature. The experiments were performed in a three-phase liquid-liquid-solid (L (oil) –L (solvent) –S (catalyst)) system, acetonitrile was used as solvent and dodecane as oil phase. Solution samples were recovered at various times. The products were analyzed by GC HP 5890 Series II with a HP-5 column and connected to FID and PFPD detectors, after filtration and eventually decantation step. The products were confirmed using a Shimadzu GCMS. Structural and textural characterization of the titanium modified-mesoporous carbon was performed by N2 adsorption, XRD, UV-Vis-DRS, XPS, Raman spectroscopy and TEM. The characterization results indicated that the textural and structural properties of the material synthesized by the short time method are comparable with the properties of the material prepared by the hard template method. Ti modified-mesoporous carbon was synthesized by different methods in order to prepare catalysts to be tested in the oxidative desulfurization (ODS) of sulfur compounds. The good performance and stability of the catalyst prepared using a novel synthesis method was attributed to well dispersed anatase nanospecies over the high area mesoporous carbon. Main advantage of the present study is the reduction of time and cost in the synthesis of the new material and the applicability for ODS reactions.Item Novel preparation of titania-modified CMK-3 nanostructured material as support for Ir catalyst applied in hydrodenitrogenation of indole.(Univesidsad Tecnológica Nacional., 2018) Ledesma , Brenda Cecilia; Juárez , Juliana María; Vallés , Verónica Alejandra; Anunziata , Oscar Alfredo; Beltramone , Andrea Raquel; Anunziata , Oscar Alfredo; Vallés , Verónica Alejandra; Juárez , Juliana MaríaIridium catalyst was prepared using a novel titanium oxide-CMK-3 support synthesized as a replica of Ti-SBA-15. The catalyst was applied in the hydrodenitrogenation of indole. The activity was compared with an iridium catalyst supported over a grafted titanium CMK-3. Structural and textural characterization of the catalysts was performed by means of N2 adsorption, XRD, UV–Vis–DRS, Raman spectroscopy, XPS, TEM and H2 Chemisorption. Ir-Ti-CMK-3 was the most active catalyst for the hydrodenitrogenation reaction at mild conditions. Titanium oxide contained in carbon ordered mesoporous CMK-3 promotes a very good anchorage of iridium metallic clusters in the carbon framework reaching high active site distribution and more stable nanoclustersItem Sulfur elimination by ODSwith titanium-modified SBA-16.(Univesidsad Tecnológica Nacional., 2015) Rivoira , Lorena Paola; Vallés , Verónica Alejandra; Ledesma , Brenda Cecilia; Martínez , María Laura; Anunziata , Oscar Alfredo; Beltramone, Andrea RaquelOver the past, oxidative desulfurization (ODS) has drawn considerable interest as a new alter-native method for deep sulfur elimination from light oils. This can be attributed to its attractive properties, including lower temperature and pressure conditions and lower operating cost than conventional hydrodesulfurization (HDS) process. Oxidation of organosulfur compounds results in the formation of sulfoxides/sulfones, highly polar and hence easily removed by both extraction into polar solvents or by adsorption. Due to their low reactivity, dibenzothiophene derivatives (DBTs) are the most refractory species to be eliminated from oils. Hence, the ODS process through which DBTs are converted to their corresponding sulfones involves great interest at present. In this work, we describe the preparation and characterization of new mesoporous catalytic materials based on Ti-containing SBA-16. We study here, the effect of the preparation method of titania-modified SBA-16 (characteristics of the active Ti and/or TiO2 species) and the effect of the different operation conditions in ODS of DBT under mild conditions in order to find the best performance. TiO2-modified mesoporous SBA-16 and titanium-substituted mesoporous SBA-16 were developed and tested in the oxidative desulfurization (ODS) of dibenzothiophene prevailing in liquid fuel. We assessed the impact exerted on performance of different reaction variables, including (nature and amount of the active catalytic species, phase system, molar ratio of oxidant H2O2 and DBT, reaction temperature, nature of the substrate and reuse of catalysts). We achieved 90% of S removal from a 0.2 wt.% dibenzothiophene solution at 60°C in less than 1 h of reaction. The best catalytic results are obtained with high exposed surface of nanometric TiO2 species of TiO2/SBA-16 sample. The activated catalyst is very active in ODS reaction and can be reused four times with no loss in activity