UTN- FRC -Producción Académica de Investigación y Desarrollo
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Item Sulfated/Zr-containing mesoporous carbons: a promising nanostructured catalytic material.(Univesidsad Tecnológica Nacional., 2021) Anunziata , Oscar Alfredo; Martínez , María Laura; Martínez , María LauraIn this work, we report the successful preparation of a promising material with acidic properties from starch-derived mesoporous carbon (SMC), functionalized with sulfated zirconia (SZr-SMC). The process of assembling P123, starch, zirconia, and silicon produces ordered mesoporous carbon modified with Zr. Reaction time and temperature are essential to avoid the appearance of poorly assembled or unsightly structures, reducing the surface area and the size of the pores. SZr- SMC has a surface area of approximately 1300 m2/g, and a total pore volume of 0.94 cm3/g, composed mainly of mesoporous with an average pore size of 3.5 nm. The composition of the surface and the chemical states of the elements did not reveal ZrO2 as isolated clusters. Ammonia thermodesorption studies indicated that, SZr-SMC retains 2.49 mmol/g of NH3 at very high temperature, exhibiting a strong acidity. According to the data collected by infrared spectroscopy (FTIR), of pyridine desorbed at various temperatures, the total number of acidic sites was 2.36 mmol/g, and the distribution in weak - medium, strong, and super acidic sites was determined. The activity in the methylation of aniline and isopropanol dehydration indicated that the acid sites are strong, and have not redox properties. A new and promising catalytic material based on mesoporous carbons modified with sulfated Zr is developed, which opens a wide range of acid-catalyzed reactions applied to industrial and medical processes.Item HaP/SBA-3 Nanostructured Composite to Remove Fluoride Effectively from Contaminated Water.(Univesidsad Tecnológica Nacional., 2021) Cussa , jorgelina; López, Claudia; Anunziata , Oscar Alfredo; Anunziata , Oscar Alfredo; López, ClaudiaElectron Microscopy (SEM), Transmission Electron Microscopy (TEM) and textural properties, were successfully applied to remove fluoride from contaminated water. The proposed procedure to prepare HaP/SBA-3 was successful, which acts as supports to anchor the HaP crystals, in nanometer-scale (<2nm), with higher fluoride retention from contaminated water. The free OH- groups of HaP nanocrystals, within the host, facilitated the high-performance fluoride trapping. The fluoride retention activity was much higher than that of pure HaP and the composites HaP/SBA-15 and HaP/MCM-41. Keywords: F- retention; Contaminated water; HaP/SBA-3; NanocompositesItem Novel mesoporpous carbon modified with zirconia for hydrogen adsorption.(Univesidsad Tecnológica Nacional., 2021) Venosta, Lisandro; Juárez , Juliana María; Anunziata , Oscar Alfredo; Gómez Costa, Marcos Bruno; Anunziata , Oscar Alfredo; Juárez , Juliana MaríaNanostructured carbon material (CMK-3) modified with zirconium oxide was synthesized by a new direct synthesis technique. Zirconium oxide dispersed in carbon materials (Zr-CMK-3) were characterized by X-ray diffraction, textural properties, UV-Vis-DRS, XPS, and transmission electron microscopy analysis. The goal of this new synthesis method is to avoid the use of inorganic siliceous template (SBA-15), which leads to a shorter and cheaper way to obtain mesoporous carbon, and at the same time incorporate into the framework Zirconium atoms. Zr-CMK-3 material significantly improved H2 storage behaviour (4.6% by weight at 77 K and 10 bar) compared to CMK-3 support. The synthesized material is promising in the absorption of hydrogen by weak bonding forces (physisorption). The activity of the samples to the adsorption of hydrogen molecules is attributed to the improved dispersion of the zirconium oxide, as well as the appropriate use of support, which can probably disperse the zirconium on its large surface area, allowing a great dispersion of the zirconium. The Zr+4 cation is an active species to absorb and store hydrogen through a physisorption process and the carbon plays an important role in the dispersion and size of metal particles. A hydrogen storage mechanism on the active surface of the ZrO2 clusters was proposed. First layer of hydrogen molecules can react with the metal cation through a dihydrogen complex (Kubas interaction). The second layer of hydrogen molecules adsorbed around the metal oxide clusters is due to dipole-like interactions, this is because the metal particle induces dipole forces on the hydrogen molecule. The other layers could also interact by dipole forces; however, the interaction force decreases as the distance to the surface increases. The upper layers could interact with the metal cation by dipole-induced bonding; however, the interaction force decreases as the distance to the surface increases.Item Síntesis directa del carbón mesoporoso ordenado CMK-3 modificado con circonio en almacenamiento de energía.(Univesidsad Tecnológica Nacional., 2020) Venosta, Lisandro; Juárez , Juliana María; Anunziata , Oscar Alfredo; Gómez Costa , Marcos Bruno; Anunziata , Oscar Alfredo; Juárez , Juliana MaríaEn este trabajo, informamos la síntesis y caracterización del material de carbono nanoestructurado (CMK-3) modificado con óxido de circonio sintetizado por una nueva técnica de síntesis directa. Este material es prometedor en la aplicación de adsorción de hidrógeno para el almacenamiento de energía. Los materiales con óxido de circonio (Zr-CMK-3) se sintetizaron con éxito y se caracterizaron por difracción de rayos X, propiedades texturales, UV-Vis-DRS, XPS y análisis de microscopía electrónica de transmisión. El material Zr-CMK-3 mejoró significativamente el comportamiento de almacenamiento de H2 (4,6% en peso a 77 K y 10 bar) en comparación con el soporte CMK-3. El material sintetizado es prometedor en la absorción de hidrógeno por fuerzas de enlace débiles (fisisorción). Se propuso un mecanismo de adsorción de hidrógeno y se discutió el rol de catión Zr+4 en la absorción de hidrógeno. Palabras clave: Circonio, CMK-3, Hidrógeno, Almacenamiento, EnergíaItem Superacid Mesoporous Carbons Based on Sulfated Zr.(Univesidsad Tecnológica Nacional., 2020) Anunziata , Oscar Alfredo; Martínez , María Laura; Martínez , María LauraIn this brief communication we report the successful preparation of a promising material with acidic properties from starch-derived mesoporous carbon (SMC), functionalized with sulfated zirconia. The process of assembling P123, starch, zirconia and silicon produces ordered mesoporous carbon modified with Zr. Reaction time and temperature are essential to avoid the appearance of poorly assembled or unsightly structures, reducing the surface area and the size of the pores. Zr-SMC has a surface area of approximately 1300 m2 g -1 , and the total pore volume of 0.94 cm3 g -1 , composed mainly of mesopores with an average pore size of 3.5 nm. The composition of the surface and the chemical states of the elements did not reveal ZrO2 as isolated clusters. Through the thermodesorption of the pre adsorbed ammonia in the sulfated Zr-SMC, the total ammonia retained is 1.80 mmol / g at high temperature, exhibiting medium to strong acidity.Item HaP/LP-SBA15 Nanocomposite for efficient removal of fluoride from contaminated water.(Univesidsad Tecnológica Nacional., 2020) López, Claudia; Cussa, jorgelina; Anunziata , Oscar Alfredo; Anunziata , Oscar Alfredo; Cussa, jorgelinaHydroxyapatite (HaP) composites and highly ordered large pore mesoporous silica, such as LP-SBA 15 (Large Pore-SBA-15), were developed, characterized by XRD, BET, FTIR, and HRTEM, applied to fluoride removal from contaminated water. The proposed procedure to prepare HaP/LP-SBA-15 was successful, which acts as supports to anchor the HaP crystals, in nanometer-scale (<12 nm), with higher fluoride retention from contaminated water. The free OH- groups of HaP nanocrystals, inside the host, permitted fluoride retention with high capacity. The fluoride holding activity was over 3 orders of magnitude higher than pure HaP.Item Hydrogenation of tetralin in presence of nitrogen using a noble-bimetallic couple over a Ti-modified SBA-15.(Univesidsad Tecnológica Nacional., 2016) Vallés , Verónica Alejandra; Ledesma , Brenda Cecilia; Pecchi, Gina; Anunziata , Oscar Alfredo; Beltramone , Andrea Raquel; Anunziata , Oscar Alfredo; Ledesma , Brenda CeciliaMonometallic Pt- and bimetallic Pt-Ir-modified Ti-SBA-15 were used in the hydrogenation of tetralin to decalin in the presence of 150 ppm of N as quinoline and indole at 250 ◦C and 15 atm of pressure of hydrogen, using a Parr reactor. The catalyst was synthesized using sol-gel method and Ti was added during the synthesis using Tetraethyl Orthotitanate. Pt/Ir was added by wetness impregnation. The catalysts prepared were extensively characterized by X-ray diffraction (XRD), N2 adsorption isotherms, UV–vis DRS, Raman spectroscopy, XPS, TEM-EDS and TPR. UV–vis-DRS and Raman spectroscopy confirmed that Ti was incorporated in tetrahedral coordination in the framework of the SBA-15. The analysis showed that the mesoporous structure was maintained after metal incorporation and Ti incorporation helps to reduce significantly the size of the metals clusters and improves its dispersion considerably. Pt-Ir/Ti-SBA 15 was the most active catalyst. The experimental data were quantitatively represented by a modified Langmuir-Hinshelwood type rate equation. The preliminary results show these materials as a promising catalyst for HDT reactions.Item Experimental desing optimization of the tetralin hydrogenation over Ir-Pt-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 , Brenda CeciliaExperiment design-response surface methodology (RSM) is used in this work to model and optimize two responses in the hydrogenation of tetralin to decalin using bimetallic Ir–Pt-SBA-15 catalyst. In this study, we analyze the influence of the nature of the catalyst (metal molar fraction and metal loading), the catalyst/substrate ratio and the temperature of the reaction as factors for the design. The responses analyzed were conversion at 3 h and at 5 h 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 two objective functions were obtained employing the catalyst with 1 wt.% of iridium and 0.7–0.8 wt.% of platinum; the optimal ratio between mass of catalyst and mole of tetralin was 17–19 g/mol and temperature between 200 and 220 ◦CItem Sulfur elimination by oxidative desulfurization with titanium-modified SBA-16.(Univesidsad Tecnológica Nacional., 2015) Rivoira , Lorena Paola; Vallés , Verónica Alejandra; Ledesma , Brenda Cecilia; Ponte , María Virginia; Martínez , María Laura; Anunziata , Oscar Alfredo; Beltramone, Andrea Raquel; Anunziata , Oscar Alfredo; Martínez , María Laura; Ponte , María Virginia; Ledesma , Brenda Cecilia; Vallés , Verónica AlejandraTiO2-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. Pure TiO2 was used as reference. The titania-based catalysts were characterized by chemical analysis, XRD, EDX and TEM. The titanium state as tetrahedral (in Ti-SBA-16 sample) or octahedral (in TiO2/SBA-16 sample) coordination surrounding in the silicate matrix was determined by XPS, UV–vis DRS, FTIR, Raman and XANES. 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). In addition, we carried out a kinetic study and the activation energy was determined. 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.Item Optimization of the synthesis of SBA-3 mesoporous materials by experimental desing.(Univesidsad Tecnológica Nacional., 2015) Ponte , María Virginia; Rivoira , Lorena Paola; Cussa , jorgelina; Martínez , María Laura; Beltramone , Andrea Raquel; Anunziata , Oscar Alfredo; Anunziata , Oscar Alfredo; Anunziata; Cussa , jorgelina; Rivoira , Lorena PaolaSBA-3 mesoporous materials are characterized by hexagonal regular arrangements of channels with diameters >2 nm, high specific surface areas and high specific pore volumes. In the work reported herein, experimental design-response surface methodology (RSM) is used to model and optimize the synthesis conditions for SBA-3 mesoporous materials. In this study, we evaluate the influences of surfactant/silica source molar ratios, aging times, temperature and pH on the synthesis of SBA-3 mesoporous materials by analyzing the XRD intensities pertaining to the [100] signal. Response surfaces were obtained using the BoxeBehnken design, and the combination of reaction parameters was optimized. By applying statistical methodology, higher levels of the objective function (XRD intensities pertaining to the [100] signal) were obtained using cetyltrimethylammonium bromide (CTAB)/tetraethyl orthosilicate (TEOS) molar ratios of 0.07 and 0.16, HCl/TEOS molar ratios of 8 and 11, reaction temperatures of 35 and 45 ◦C and aging times of 12e24 h. The mesoporous SBA-3 samples obtained were characterized using small-angle X-ray powder diffraction (XRD), BET, FTIR and 29Si NMR-MAS, scanning electron microscopy (SEM) and transmission electron microscopy (TEM).