Well-organized, spherical, mesoporous hollow @CuMgAl-LDHs (layered double hydroxides) are prepared by the controlled removal of the SiO from SiO@CuMgAl-LDH core-shell hybrids that in turn are synthesized a bottom-up strategy. The materials are prepared with various Cu/Mg molar ratios (Cu/Mg = 0.05-0.
View Article and Find Full Text PDFIn this paper, we describe the role of anatase and rutile crystal phases on diphenyl sulphide (PhS) catalytic and photocatalytic oxidation. The highly selective and efficient synthesis of diphenyl sulfoxide (PhSO) and diphenyl sulfone (PhSO) at titanium dioxide was demonstrated. PhS oxidation in the presence of hydrogen peroxide at anatase-TiO can take place both as a catalytic and photocatalytic reaction, while at rutile-TiO only photocatalytic oxidation is possible.
View Article and Find Full Text PDFFerrierites and their delaminated (ITQ-6) and silica intercalated (ITQ-36) forms, with the intended molar Si/Al ratios of zeolite layers of 30 and 50, were synthesized and tested as catalysts of methanol to dimethyl ether (DME) as well as ethanol to diethyl ether (DEE) and ethylene dehydration. It was shown that increased content of acid sites, especially of Brønsted type, resulted in more active catalysts of alcohol dehydration. Brønsted acid sites dominate in ferrierites and their delaminated forms (ITQ-6).
View Article and Find Full Text PDFTitanium-silicon ferrierites with different Si/Ti ratios and their delaminated forms were modified with copper by ion-exchange. The obtained samples were characterized with respect to their chemical composition (ICP-OES), structure (XRD), texture (N sorption), morphology (SEM), form and aggregation of titanium and copper species (UV-vis-DRS), reducibility of deposited copper species (H-TPR) and surface acidity (NH-TPD). The porous structure of the zeolitic samples strongly influenced the form and aggregation of deposited copper species.
View Article and Find Full Text PDFTwo series of strontium titanates doped with Ni, Co, or Cu with general formula of SrTiMeO for Sr-stoichiometric and SrTiMeO for Sr-non-stoichiometric materials (where Me = Ni, Co or Cu and x were 0.02 and 0.06) were obtained by the wet chemical method.
View Article and Find Full Text PDFAluminum containing silica spherical MCM-41 was synthesized and modified with copper by the template ion-exchange method (TIE) and its modified version, including treatment of the samples with ammonia solution directly after template ion-exchange (TIE-NH). The obtained samples were characterized with respect to their chemical composition (ICP-OES), structure (XRD), texture (low temperature N sorption), morphology (SEM-EDS), form and aggregation of deposited copper species (UV-vis DRS), reducibility of copper species (H-TPR), and surface acidity (NH-TPD). The deposition of copper by the TIE-NH method resulted in much better dispersion of this metal on the MCM-41 surface comparing to copper introduced by TIE method.
View Article and Find Full Text PDFSpherical MCM-41 with various copper and iron loadings was prepared by surfactant directed co-condensation method. The obtained samples were characterized with respect to their structure (X-ray diffraction, XRD), texture (N sorption), morphology (scanning electron microscopy, SEM), chemical composition (inductively coupled plasma optical emission spectrometry, ICP-OES), surface acidity (temperature programmed desorption of ammonia, NH-TPD), form, and aggregation of iron and copper species (diffuse reflectance UV-Vis spectroscopy, UV-Vis DRS) as well as their reducibility (temperature programmed reduction with hydrogen, H-TPR). The spherical MCM-41 samples modified with transition metals were tested as catalysts of selective catalytic reduction of NO with ammonia (NH-SCR).
View Article and Find Full Text PDFFerrierites and their delaminated forms (ITQ-6), containing aluminum or titanium in the zeolite framework, were synthetized and modified with copper by an ion-exchange method. The obtained samples were characterized with respect to their chemical composition (ICP-OES), structure (XRD, UV-Vis DRS), textural parameters (N-sorption), surface acidity (NH-TPD), form and reducibility of deposited copper species (UV-Vis DRS and H-TPR). Ferrierites and delaminated ITQ-6 zeolites modified with copper were studied as catalysts for the selective catalytic oxidation of ammonia to dinitrogen (NH-SCO).
View Article and Find Full Text PDFMCM-22, MCM-36, and ITQ-2 zeolites with the intended Si/Al molar ratios of 15, 25, and 50 were synthetized and tested as catalysts for dehydration of methanol to dimethyl ether and dehydration of ethanol to diethyl ether and ethylene. The surface concentration of acid sites was regulated by the synthesis of zeolite precursors with different aluminum content in the zeolite framework, while the influence of porous structure on the overall efficiency of alcohol conversion was analyzed by application of zeolitic materials with different types of porosity-microporous MCM-22 as well as microporous-mesoporous MCM-36 and ITQ-2. The zeolitic samples were characterized with respect to their: chemical composition (ICP-OES), structure (XRD, FT-IR), texture (N sorption), and surface acidity (NH-TPD).
View Article and Find Full Text PDFSamples of TiO (P25) doped with zinc, tin, and vanadium, thermally treated at 550 °C for 6 h, were tested as catalysts and photocatalysts for the oxidation of diphenyl sulphide to diphenyl sulfoxide and sulfone, using hydrogen peroxide as an oxidation agent. Thermal treatment of pure TiO and its vanadium-doped forms resulted in a decrease of anatase and an increase of rutile content. The opposite effect was observed for TiO doped with zinc or tin, where thermal treatment resulted in the rutile to anatase phase transition.
View Article and Find Full Text PDFVarious temperature-programmed techniques were used as tools in mechanistic studies of selective catalytic reduction (SCR) of NO with ammonia in the presence of Fe-containing BEA zeolites. Moreover, FTIR studies of adsorbed NH and NO were conducted to determine the interactions of reactants with the catalyst surface. Iron was introduced into BEA zeolite by three different methods: i) two-step post-synthesis; ii) conventional wet impregnation; iii) ion exchange.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
May 2018
Two-step preparation of iron and cobalt-containing MCM-56 zeolites has been undertaken to evaluate the influence of their physicochemical properties in the selective catalytic reduction (NH-SCR or DeNOx) of NO using NH as a reductant. Zeolites were prepared by the selective leaching of the framework cations by concentrated HNO solution and NHF/HF mixture and consecutively, introduction of Co and Fe heteroatoms, in quantities below 1wt%. Further calcination allowed to obtain highly dispersed active species.
View Article and Find Full Text PDFIron-substituted MFI, Y and USY zeolites prepared by two preparation routes-classical ion exchange and the ultrasound modified ion-exchange method-were characterised by micro-Raman spectroscopy, X-ray diffraction (XRD), scanning electron microscopy (SEM), and ultraviolet (UV)/visible diffuse reflectance spectroscopy (UV/Vis DRS). Ultrasound irradiation, a new technique for the preparation of the metal salt suspension before incorporation to the zeolite structure, was employed. An experimental study of selective catalytic reduction (SCR) of NO with NH₃ on both iron-substituted reference zeolite catalysts and those prepared through the application of ultrasound conducted during an ion-exchange process is presented.
View Article and Find Full Text PDFAdditional treatment with NaOH of acid activated vermiculite results in even higher increase in the adsorption capacity in comparison to samples modified only in acidic solution (first step of activation) with respect to raw material. Optimization of treatment conditions and adsorption capacity for two cationic dyes (methylene blue (MB) and astrazon red (AR)), also as binary mixture, was evaluated. The capacity, based on column studies, increased from 48 ± 2 to 203 ± 4 mg g in the case of methylene blue and from 51 ± 1 to 127 ± 2 mg g in the case of astrazon red on starting and acid-base treated material, respectively.
View Article and Find Full Text PDFThe aim of this work was the modification of vermiculite in order to produce a low cost, efficient and sustainable adsorbent for dyes and metals. Three activation methods consisting of acid, base and combined acid/base treatment were applied to improve the of vermiculite's adsorption properties. Adsorbents were tested in single, bi- and tricomponent solutions containing cationic dyes and Cu cations.
View Article and Find Full Text PDFNickel and sulfur doped lithium manganese spinels with a nominal composition of LiMnNiOS (0.1 ≤ ≤ 0.5 and = 0.
View Article and Find Full Text PDFThe influence of different acid treatments over vermiculite was evaluated. Equilibrium, kinetic and column studies have been conducted. The results showed that vermiculite first treated with nitric acid and then with citric acid has higher adsorption capacity, presenting maximum adsorption capacities in column experiments: for Astrazon Red (AR), 100.
View Article and Find Full Text PDFSupported vanadium and titanium oxide catalysts were prepared by adsorption and subsequent calcination of the vanadyl and titanyl acetylacetonate complexes, respectively, on mesoporous SBA-15 by the molecular designed dispersion (MDD) method. Liquid and gas phase depositions at different temperatures were carried out with vanadyl acetylacetonate, and the different results together with those of titanyl acetylacetonate in the liquid phase deposition were discussed. The bonding mechanism, the influence of the metal interaction with the support material, and differences due to the way of deposition and the temperature were investigated by TGA, chemical analysis, FTIR, and Raman spectroscopy.
View Article and Find Full Text PDFFour various mesoporous silicas (MCM-48, SBA-15, MCF, and MSU) were modified by the molecular designed dispersion method using Fe(acac)3, Cr(acac)3, and Cu(acac)2 complexes. The deposition was performed at the same concentration of the metal acetylacetonate (acac) complex in a toluene solution. All as-synthesized samples were investigated by diffuse reflectance infrared Fourier transform spectroscopy, Fourier transform infrared photoacoustic spectroscopy, and thermogravimetric analysis.
View Article and Find Full Text PDFThe novel mesoporous templated silicas (MCM-48, SBA-15, MCF, and MSU) were used as supports for transition metal (Cu, Cr, or Fe) oxides. The catalysts were synthesized using the incipient wetness impregnation, and characterized by low-temperature N2 sorption, DRIFT, photoacoustic IR spectroscopy, UV-vis diffuse reflectance spectroscopy, and temperature-programmed desorption of ammonia. It was shown that the preparation method used results in different distributions and dimensions of the transition metal oxide clusters on the inert support surface.
View Article and Find Full Text PDFMCM-48, SBA-15, MCF, and MSU mesoporous silicas were used as supports for a deposition of Fe oxide species. Iron was introduced using two different methods: the wetness impregnation and the molecular designed dispersion (MDD). The obtained catalysts were characterized with respect to their textural parameters (BET), chemical composition (electron microprobe analysis), and reducibility (TPR).
View Article and Find Full Text PDFVanadium oxide was deposited on mesoporous titania by the molecular designed dispersion method to investigate the potential properties of these catalysts. Mesoporous titania was synthesized following the evaporation-induced self-assembly (EISA) method with a subsequent treatment with ammonia to increase the thermal stability. As a result, the mesoporous titania obtained shows a high surface area (approximately 350 m2/g) and high stability.
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