Open Access
Photocatalytic degradation of trimethoprim on doped Ti-pillared montmorillonite
(Elsevier, 2019) González, Beatriz; Trujillano, Raquel; Vicente, Miguel Ángel; Rives, Vicente; Korili, Sophia A.; Gil Bravo, Antonio; Institute for Advanced Materials and Mathematics - INAMAT2
Montmorillonite pillared with titanium and doped with Cr3+ or Fe3+ has been tested for the photo-degradation of the antibiotic trimethoprim (trimethoxybenzyl-2,4-pyrimidinediamine) under different conditions, namely, in the dark or in UV light, with or without catalyst, finding excellent catalytic performance under photocatalytic conditions. The degradation by-products were preliminary analysed by mass spectrometry. The results suggested that the molecule broke in two halves, corresponding to its two existing rings. The process continued with the breakage of new fragments from the trimethoxybenzene half, these fragments later reacted with the methoxy groups in this part of the molecule, giving species with m/z values higher than that for the starting molecule, and with the breakage of new fragments.
Open Access
Microwave-assisted pillaring of a montmorillonite with al-polycations in concentrated media
(MDPI, 2017) González, Beatriz; Pérez, Alba Helena; Trujillano, Raquel; Gil Bravo, Antonio; Vicente, Miguel Ángel; Química Aplicada; Kimika Aplikatua
A montmorillonite has been intercalated with Al3+ polycations, using concentrated solutions and clay mineral dispersions. The reaction has been assisted by microwave radiation, yielding new intercalated solids and leading to Al-pillared solids after their calcination at 500 °C. The solids were characterized by elemental chemical analysis, X-ray diffraction, FTIR spectroscopy, thermal analyses, and nitrogen adsorption. The evolution of the properties of the materials was discussed as a function of the preparation conditions. Microwave treatment for 2.5 min provided correctly pillared solids.
Open Access
Application of industrial wastes from chemically treated aluminum saline slags as adsorbents
(American Chemical Society, 2018) Gil Bravo, Antonio; Arrieta Chango, Ekhine; Vicente, Miguel Ángel; Korili, Sophia A.; Institute for Advanced Materials and Mathematics - INAMAT2
In this study, industrial wastes, which remain after aluminum extraction from saline slags, were used as adsorbents. The aluminum saline slags were treated under reflux with 2 mol/dm3 aqueous solutions of NaOH, H2SO4, and HCl for 2 h. After separation by filtration, aqueous solutions containing the extracted aluminum and residual wastes were obtained. The wastes were characterized by nitrogen adsorption at -196 °C, X-ray diffraction, scanning electron microscopy, and ammonia pulse chemisorption. The chemical treatment reduced the specific surface area, from 84 to 23 m2/g, and the pore volume, from 0.136 to 0.052 cm3/g, of the saline slag and increased the ammonia-adsorption capacity from 2.84 to 5.22 cm3/g, in the case of acid-treated solids. The materials were applied for the removal of Acid Orange 7 and Acid Blue 80 from aqueous solutions, considering both single and binary systems. The results showed interesting differences in the adsorption capacity between the samples. The saline slag treated with HCl rapidly adsorbed all of the dyes present in solution, whereas the other materials retained between 50 and 70% of the molecules present in solution. The amount of Acid Orange 7 removed by the nontreated material and by the material treated with NaOH increased in the presence of Acid Blue 80, which can be considered as a synergistic behavior. The CO2 adsorption of the solids at several temperatures up to 200 °C was also evaluated under dry conditions. The aluminum saline slag presented an adsorption capacity higher than the rest of treated samples, a behavior that can be explained by the specific sites of adsorption and the textural properties of the solids. The isosteric heats of CO2 adsorption, determined from the Clausius-Clapeyron equation, varied between 1.7 and 26.8 kJ/mol. The wastes should be used as adsorbents for the selective removal of organic contaminants in wastewater treatment.
Open Access
Effective degradation of methylene blue in aqueous solution using Pd-supported Cu-doped Ti-pillared montmorillonite catalyst
(Elsevier, 2019) Joseph, Annu; Vellayan, Kannan; González, Beatriz; Vicente, Miguel Ángel; Gil Bravo, Antonio; Institute for Advanced Materials and Mathematics - INAMAT2
The effluents from the textile, paper and food industries contain organic dyes that are strongly colored and reveal harmful effect on living systems. In order to reduce water pollution, the degradation of dye into non toxic form is desirable. Methylene blue is one such organic dye, discharged from textile industries. In this work, the catalytic degradation of methylene blue was investigated using a montmorillonite supported trimetallic catalyst, prepared by supporting Pd on a Cu-doped Ti pillared montmorillonite. The catalyst exhibited excellent performance to reduce methylene blue, in the presence of NaBH4. The decolorization was appreciable and the results indicated that methylene blue could be successfully decolorized and degraded using the catalyst under room conditions. Almost complete degradation was achieved within 20 min. The results obtained were better than those reported for other catalysts. © 2018 Elsevier B.V.
Open Access
Effect of high pressure on the reducibility and dispersion of the active phase of Fischer-Tropsch catalysts
(MDPI, 2019) Yunes, Simón; Vicente, Miguel Ángel; Korili, Sophia A.; Gil Bravo, Antonio; Zientziak; Institute for Advanced Materials and Mathematics - INAMAT2; Ciencias
The effect of high pressure on the reducibility and dispersion of oxides of Co and Fe supported on -Al2O3, SiO2, and TiO2 has been studied. The catalysts, having a nominal metal content of 10 wt.%, were prepared by incipient wetness impregnation of previously calcined supports. After drying at 60 °C for 6 h and calcination at 500 °C for 4 h, the catalysts were reduced by hydrogen at two pressures, 1 and 25 bar. The metal reduction was studied by temperature-programmed reduction up to 750 °C at the two pressures, and the metal dispersion was measured by CO chemisorption at 25 °C, obtaining values between 1% and 8%. The physicochemical characterization of these materials was completed by means of chemical analysis, X-ray diffraction, N2 adsorption-desorption at -196 °C and scanning electron microscopy. The high pressure lowered the reduction temperature of the metal oxides, improving their reducibility and dispersion. The metal reducibility increased from 42%, in the case of Fe/Al2O3 (1 bar), to 100%, in the case of Fe/TiO2 (25 bar).
Embargo
Effect of the preparation method and metal content on the synthesis of metal modified titanium oxide used for the removal of salicylic acid under UV light
(Taylor & Francis, 2018) Santamaría Arana, Leticia; Vicente, Miguel Ángel; Korili, Sophia A.; Gil Bravo, Antonio; Institute for Advanced Materials and Mathematics - INAMAT2
Titanium dioxide modified with Ag and Fe was synthesized using two preparation methods, characterized and applied to the photocatalytic degradation of salicylic acid in aqueous solution. The modified TiO2 samples were prepared by the sol–gel and wet impregnation methods starting from titanium(IV) isopropoxide and using AgNO3 and Fe(NO3)3·9H2O as precursors of the modifiers, with their content varying between 0 and 5 wt.%. Catalysts characterization was based on powder X-ray diffraction (PXRD), nitrogen physisorption at 77 K, temperature programmed reduction (H2-TPR), chemisorption of NH3 at 343 K and X-ray photoelectron spectroscopy (XPS). The photocatalytic degradation of salicylic acid by modified TiO2 was investigated under ultraviolet irradiation at 298 K considering various concentrations of the catalyst, between 100 and 1000 mgcatalyst/dm3, and of the organic molecule, between 0 and 15 mg/dm3. The catalysts most active in the degradation of salicylic acid were those having the highest Fe content. © 2018, © 2018 Informa UK Limited, trading as Taylor & Francis Group.
Open Access
Preparation of Al/Fe-pillared clays: effect of the starting mineral
(MDPI, 2017) Muñoz Alvear, Helir Joseph; Blanco, Carolina; Gil Bravo, Antonio; Vicente, Miguel Ángel; Galeano, Luis Alejandro; Química Aplicada; Kimika Aplikatua
Four natural clays were modified with mixed polyoxocations of Al/Fe for evaluating the effect of the physicochemical properties of the starting materials (chemical composition, abundance of expandable clay phases, cationic exchange capacity and textural properties) on final physicochemical and catalytic properties of Al/Fe-PILCs. The aluminosilicate denoted C2 exhibited the highest potential as starting material in the preparation of Al/Fe-PILC catalysts, mainly due to its starting cationic exchange capacity (192 meq/100 g) and the dioctahedral nature of the smectite phase. These characteristics favored the intercalation of the mixed (Al13􀀀x/Fex)7+ Keggin-type polyoxocations, stabilizing a basal spacing of 17.4 Å and high increase of the BET surface (194 m2/g), mainly represented in microporous content. According to H2-TPR analyses, catalytic performance of the incorporated Fe in the CatalyticWet Peroxide Oxidation (CWPO) reaction strongly depends on the level of location in mixed Al/Fe pillars. Altogether, such physicochemical characteristics promoted high performance in CWPO catalytic degradation of methyl orange in aqueous medium at very mild reaction temperatures (25.0 1.0 C) and pressure (76 kPa), achieving TOC removal of 52% and 70% of azo-dye decolourization in only 75 min of reaction under very low concentration of clay catalyst (0.05 g/L).