Desarrollo, Producción e Innovación en la Investigación científica
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Item Experimental desing optimization of the ods of DBT using V2O5 supported on GA-SBA-15.(Univesidsad Tecnológica Nacional., 2020) Rivoira , Lorena Paola; Cussa , jorgelina; Martínez , María Laura; Beltramone , Andrea Raquel; Martínez , María Laura; Cussa , jorgelinaExperiment design-response surface methodology (RSM) was used in this work to model and optimize one response in the oxidative desulfurization of dibenzothiophene with hydrogen peroxide using VOx Ga-SBA-15 catalysts with different Ga/Si and V/Si ratios. In this study, we analyze the influence of the nature of the catalyst (metal/Si ratio), the substrate/catalyst mass ratio and the oxidant/substrate ratio as factors for the design. The response analyzed was conversion at 15 min of reaction time. The response surfaces were obtained with the Box– Behnken Design, finding the best combination between the reaction parameters that allowed optimizing the process. By applying the statistic methodology, the higher levels of the objective function were obtained employing the catalyst with 4 wt.% of gallium and 6 wt.% of vanadium; the optimal ratio between g DBT/g of catalyst was 4 and the molar ratio H2O2/DBT was 5. The incorporation of gallium as heteroatom in tetrahedral position allows the better anchorage of the active species of vanadium generating a very well dispersed catalyst. Structural and textural characterization of the catalysts were performed by means of XRD, N2 adsorption, UV–Vis–DRS, XPS, NMR, TEM, Raman, TPR and Py-FTIR. UV–Vis–DRS and Raman demonstrated that highly dispersed vanadium pentoxide crystallites are responsible for the high activity in the sulfur removal. The high dispersion depended on the vanadium loading and on the nature of the support. The experiment design was able to find the best combination between the heteroatom and the vanadium active site in order to find the most active catalyst for ODS of DBT at the optimized experimental conditions.Item Experimental Desing Optimization of the ODS of DBT using V2O5 supported on Ga-SBA-15.(Univesidsad Tecnológica Nacional., 2020) Rivoira , Lorena Paola; Cussa , jorgelina; Martínez , María Laura; Beltramone , Andrea Raquel; Martínez , María Laura; Cussa , jorgelinaExperiment design-response surface methodology (RSM) was used in this work to model and optimize one response in the oxidative desulfurization of dibenzothiophene with hydrogen peroxide using VOx-Ga-SBA-15 catalysts with different Ga/Si and V/Si ratios. In this study, we analyze the influence of the nature of the catalyst (metal/Si ratio), the catalyst/substrate ratio and the oxidant/substrate ratio as factors for the design. The response analyzed was conversion at 15 min of reaction time. The response surfaces were obtained with the Box–Behnken Design, finding the best combination between the reaction parameters that allowed optimizing the process. By applying the statistic methodology, the higher levels of the objective function were obtained employing the catalyst with Ga/Si and V/Si ratios of v1/15 and 1/25, respectively. Structural and textural characterization of the catalysts were performed by means of XRD, N2 adsorption, UV–Vis–DRS, XPS, NMR, TEM, Raman, TPR and Py-FTIR. UV–Vis–DRS and Raman demonstrated that highly dispersed vanadium pentoxide crystallites are responsible for the high activity in the sulfur removal. The high dispersion depended on the vanadium loading and on the nature of the support.Item Experimental desing optimization of the ODS of DBT using V2O5 supported on GA-SBA-15.(Univesidsad Tecnológica Nacional., 2020) Rivoira , Lorena Paola; Cussa , jorgelina; Martínez , María Laura; Beltramone, Andrea Raquel; Martínez , María Laura; Cussa , jorgelinaExperiment design-response surface methodology (RSM) was used in this work to model and optimize one response in the oxidative desulfurization of dibenzothiophene with hydrogen peroxide using VOx Ga-SBA-15 catalysts with different Ga/Si and V/Si ratios. In this study, we analyze the influence of the nature of the catalyst (metal/Si ratio), the substrate/catalyst mass ratio and the oxidant/substrate ratio as factors for the design. The response analyzed was conversion at 15 min of reaction time. The response surfaces were obtained with the Box– Behnken Design, finding the best combination between the reaction parameters that allowed optimizing the process. By applying the statistic methodology, the higher levels of the objective function were obtained employing the catalyst with 4 wt.% of gallium and 6 wt.% of vanadium; the optimal ratio between g DBT/g of catalyst was 4 and the molar ratio H2O2/DBT was 5. The incorporation of gallium as heteroatom in tetrahedral position allows the better anchorage of the active species of vanadium generating a very well dispersed catalyst. Structural and textural characterization of the catalysts were performed by means of XRD, N2 adsorption, UV–Vis–DRS, XPS, NMR, TEM, Raman, TPR and Py-FTIR. UV–Vis–DRS and Raman demonstrated that highly dispersed vanadium pentoxide crystallites are responsible for the high activity in the sulfur removal. The high dispersion depended on the vanadium loading and on the nature of the support. The experiment design was able to find the best combination between the heteroatom and the vanadium active site in order to find the most active catalyst for ODS of DBT at the optimized experimental conditions.Item Tetralin hydrogenation over Ir-Pt/SBA-15. optimization by experimental desing.(Univesidsad Tecnológica Nacional, 2024) Vallés , Verónica Alejandra; Ledesma, Brenda Cecilia; Rivoira, Lorena Paola; Cussa , jorgelina; Anunziata , Oscar Alfredo; Beltramone , Andrea Raquel; Anunziata , Oscar Alfredo; 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 Preparation and characterization of activated CMK-3 modified with vanadium applied in hydrogen storage.(Univesidsad Tecnológica Nacional, 2024) Juárez , Juliana María; Gómez Costa, Marcos Bruno; Cussa , jorgelina; Anunziata , Oscar Alfredo; Anunziata , Oscar Alfredo; Cussa , jorgelinaThe aim of this work is to synthesize a nanostructured Carbon CMK-3 modified with V in order to increase its capacity in hydrogen storage. The approach that we have followed includes synthesis of nanostructures with the experimental study of its adsorption capacity and storage properties. Ordered nanoporous carbon CMK-3 was synthesized via a two-step impregnation of the SBA-15 mesopores with a solution of sucrose using an incipient wetness method. The sucrose–silica composite was heated at 1173 K for 4 h under nitrogen flow. The silica template was dissolved with 5 wt% hydrofluoric acid in order to remove the silica. The template-free carbon product thus obtained was filtered, washed with deionized water and ethanol, and dried. [1] V-CMK-3 was prepared by wetness impregnation using VCl3 as source of Vanadium in order to increase the amount of hydrogen adsorbed. The sample of V-CMK-3 was treated under H2 flow two times at 1173 K. Porous carbon CMK-3 and the sample modified with V were characterized by XRD, FTIR, XPS, BET, TEM and SEM. These studies indicate that it was possible to obtain a CMK-3 replica successfully from SBA-15, using sucrose as a carbon precursor. [2] The surface areas are 1320 m2/g and 1050 m2/g for CMK-3 and V-CMK-3, respectively. While the nanomaterial area is significantly smaller with the incorporation of the metal, CMK-3`s characteristic structure is maintained after the metal is within the host, in agreement with the XRD studies. Measurements of hydrogen adsorption at cryogenic temperatures and low pressures were performed. The nanoparticles of V incorporated onto the nanostructured carbon CMK-3 showed higher hydrogen uptake at low and high pressures than CMK-3. (3.4 wt% and 2.2 wt% respectively of H2 sorption at 10 bar and 77 K).Item Synthesis, characterization and catalytic performance of bimetallic Ir-Pt catalysts for tetralin hydrogenation.(Univesidsad Tecnológica Nacional, 2024) Anunziata , Oscar Alfredo; Beltramone, Andrea RaquelBimetallic Pt–Pd catalysts have received considerable attention, because they show high activity in a variety of catalytic applications (1) and stability compared with monometallic Pt or Pd catalysts. For instance, the bimetallic Pt–Pd catalysts have been shown to have higher resistance toward poisonscompared to Pt catalysts (2-4). For supported bimetallic clusters, the surface and bulk composition strongly depend on a series of parameters, for example, preparation procedures, metal–metal and metal–support interactions. The final goal is to find the optimal proportion of each metal in order to be more active in these processes.In this case a series of Ir and Pt modified SBA-15 were prepared by the consecutive wet impregnation method, with different content of each metal. The final catalysts were characterized by XRD, TEM and H2 chemisorption to study the effect of content of metal on the dispersion of iridium/platinum. The catalysts synthesized with similar percentage of both metal showed the best activity measured in tetralin hydrogenation. Platinum (Pt) and Iridium (Ir) nanoparticles were incorporated into SBA-15 support [1-4] by the wet co-impregnation method. The metal precursors were Iridium acetylacetonate and cloroplatinic acid. The samples were calcined at 500°C and previous to the catalytic test the samples were reduced by heating at 2°C/min to 450°C in a H2 stream for 5 h. Hereinafter this catalyst will be referred as Ir-Pt- SBA-15 (x), with x= 1-3. The catalytic activity was measured in a 4563Parr reactor, at 250°C, 15 atm of pressure of hydrogen and 360 rpm for tetralin hydrogenation (feed consisted in 50 mL of 5% v/v of tetralin (98.5% FLUKA) in Dodecane). The Pt-Ir-SBA-15 catalyst with 1 %wt. of each metals had the highest activity measured in tetralin hydrogenation at mild conditions. The good activity was correlated with higher Ir/Pt dispersion on SBA-15 mesostructured material used as support, as we seen by TEM and H2 Chemisorption, with higher active metal sites exposed to reactant. The Ir-Pt-SBA-15 activity is sufficiently high to envisage use in the final stages of a refinery process producing diesel fuel of high Cetane Number by hydrodearomatization.Item Multiple-wall carbon nanotubes obtained with mesoporous material decorated with caria-zirconia.(Univesidsad Tecnológica Nacional, 2020) Rodríguez , Miguel Angel; Anunziata , Oscar Alfredo; Beltramone, Andrea Raquel; Juárez , Juliana María; Juárez , Juliana María; Anunziata , Oscar AlfredoIn this work, Ceria-Zirconia on ordered Santa Barbara mesoporous silica (Ce-Zr-SBA-15), has been used directly as a catalyst for the synthesis of carbon nanotubes (CNTs) through Chemical Vapor Deposition (CVD). In addition to cerium oxide, it contains zirconium oxide nano crystallites, which act as catalysts for carbon nanostructures. The catalytic performance of this material was evaluated for the decomposi- tion of ethanol at 900 °C, with N2 flow. The carbon decomposed from absolute ethanol diffuses through the surface of the nanostructured catalytic material and precipitates in the form of MWCNT structures, which could be identified by X-ray diffraction (XRD), Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy (TEM), showing average diameters of 30–35 nm.Item Mesoporous Cellular Foam (MCF): an efcient and biocompatible nanomaterial for the controlled release of Chlorambucil.(Univesidsad Tecnológica Nacional, 2022) Juárez , Juliana María; Cussa , jorgelina; Gómez Costa, Marcos BrunoNanotransporters have entered a great deal of exploration attention because of their promising openings in medicine delivery. We propose in this work, the Mesostructured siliceous cellular (MCFs) nanomaterial as a promising new hostfor drug delivery systems because both their specific physicochemical properties, in addition to the high biocompatibility, biodegradability, and low toxicity, make them seductive for controlled medicine release operations. Chlorambucil, is used as a chemotherapy drug administered for treating some types of cancer, chronic lymphocytic leukemia, low-grade non Hodgkin’s lymphoma, Hodgkin’s lymphoma and ovarian cancer. Chlorambucil-loaded Mesostructured cellular foam (MCF-CLB) was prepared and characterized by XRD, TEM, UV Vis DRS, FTIR, and texture analysis determining the adsorption capacity and its release, achieving the required therapeutic efficacy. The release of the drug was conducted by simulating the physiological conditions to reproduce the conditions of the organism. The mechanism of drug release from the MCF-CLB host was evaluated. Different mathematical models were used to adjust the experimental data, the best model describing the phenomenon under study over the entire period is the Weibull model. The auspicious results we attained for the release of the drug using the new material. The main advantage of this release is that the rate of release is fast at the beginning and then gradually decreases until 24 h practically all the drug contained in the carrier is released (>95%).Item H2 storage using Zr-CMK-3 developed by a new synthesis method.(Univesidsad Tecnológica Nacional, 2021) Juárez , Juliana María; Venosta , Lisandro; Anunziata, Oscar Alfredo; Gómez Costa , Marcos Bruno; Anunziata, Oscar AlfredoOne of the biggest problems in using hydrogen as an alternative fuel is that its storage must be safe and portable. This work addresses a new direct synthesis technique used to obtain a novel mesoporous carbon (CMK-3) modified with zirconium oxide. This novel material shows promise for hydrogen adsorption and storage application for energy harvesting. Zirconium oxide (Zr-CMK-3) material is achieved through successful synthesis and characterized by XRD, SEM,Raman, BET, UV-Vis-DRS, XPS and TEM analyses. Zr-CMK-3 signifi- cantly improved H2 storage performance (reaching at 77 K and 10 bar 4.6 wt%) comparedto the pristine CMK-3. The novel material is favorable for H2 uptake by using weak bonding (physisorption). A hydrogen uptake mechanistic approach is proposed and the role of the Zr+4 cation in hydrogen adsorption is discussed.Item Synthesis and characteristics of CMK-3 modified with magnetite nanoparticles for application in hydrogen storage.(Univesidsad Tecnológica Nacional, 2020) Venosta, Lisandro; Juárez , Juliana María; Anunziata , Oscar Alfredo; Bercoff, Paula; Gómez Costa , Marcos Bruno; Anunziata , Oscar Alfredo; Juárez , Juliana María: In this work, we report the synthesis and characterization of iron oxide nanoparticles supported in nanostructured carbon (CMK-3). This material is promising in the application of hydrogen adsorption for energy storage. The material with iron oxide nano particles (Fe-CMK-3) was successfully synthesized and characterized by X-ray diffraction, textural properties analysis, transmission and scanning electron microsco py, X-ray photoelectron spectroscopy, and magnetiza tion studies. A large amount of the iron incorporated as iron oxide nanoparticles was in the magnetite phase. The incorporation of magnetite on the CMK-3 carbon surface significantly improved the storage capacity of hydrogen (4.45 wt% at 77 K and 10 bar) compared with the CMK-3 framework alone (2.20 wt% at 77 K and 10 bar). The synthesized material is promising for hy drogen adsorption by weak bond forces (physisorption). A hydrogen adsorption mechanism was proposed in which the nanoparticles of magnetite have an important role.