Examinando por Autor "Aguado, J."

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Catalytic Properties in Polyolefin Cracking of Hierarchical Nanocrystalline HZSM-5 Samples Prepared According to Different Strategies
(ELSEVIER, 2010) Serrano, David P.; Aguado, J.; Escola, J.M.; Rodríguez, J.M.; Peral, Ángel
Two series of hierarchical nanocrystalline ZSM-5 zeolites prepared by different synthesis strategies (at low temperature and from silanized seeds) and with external surface areas ranging from 150 to 250 m2 g-1 were tested in the cracking of pure LDPE and HDPE at 340ºC and of waste polyethylene at 360ºC. Hierarchical zeolites showed quite higher activity, with values even 6 times higher than a standard nanocrystalline sample used as reference (n-HZSM-5). The activity values decreased from LDPE to HDPE due to the occurrence of some degree of branching in the former polymer, which act as preferential cracking sites. The major products were C1 - C4 hydrocarbons (in the range 30 - 70%, mostly C3 - C4 olefins) and C5 - C12 hydrocarbons (20 - 60%), whose share depends on both the polyolefin and the catalyst. The amount of C13 - C40 hydrocarbons was practically negligible (< 1%) due to the high acid strength of the zeolites which promotes end-chain cracking reactions. Likewise, hierarchical nanocrystalline HZSM-5 zeolites prepared from silanized protozeolitic units showed higher activities than the hierarchical nanocrystalline HZSM-5 samples synthesized at low temperature and atmospheric pressure. The differences were especially remarkable in the case of waste polyethylene cracking. These results were ascribed to the stronger acidity of the hierarchical zeolite samples prepared from silanized seeds.
Coupling membrane separation and photocatalytic oxidation processes for the degradation of pharmaceutical pollutants
(Elsevier, 2013) Martínez, F.; López-Muñoz, M.J.; Aguado, J.; Melero, J.A.; Arsuaga, J.; Sotto, A.; Molina, R.; Segura, Y.; Pariente, M.I.; Revilla, A.; Cerro, L.; Carenas, G.
The coupling of membrane separation and photocatalytic oxidation has been studied for the removal of pharmaceutical pollutants. The retention properties of two different membranes (nanofiltration and reverse osmosis) were assessed. Comparable selectivity on the separation of pharmaceuticals were observed for both membranes, obtaining a permeate stream with concentrations of each pharmaceutical below 0.5 mg/L and a rejected flux highly concentrated (in the range of 16-25 mg/L and 18-32 mg/L of each pharmaceutical for NF-90 and BW-30 membranes, respectively), when an initial stream of six pharmaceuticals was feeding to the membrane system (10 mg/L of each pharmaceutical). The abatement of concentrated pharmaceuticals of the rejected stream was evaluated by means of heterogeneous photocatalytic oxidation using TiO2 and Fe2O3/SBA-15 in presence of hydrogen peroxide as photo-Fenton system. Both photocatalytic treatments showed remarkable removals of pharmaceutical compounds, achieving values between 80 and 100 %. The nicotine was the most refractory pollutant of all the studied pharmaceuticals. Photo-Fenton treatment seems to be more effective than TiO2 photocatalysis, as high mineralization degree and increased nicotine removal were attested. This work can be considered an interesting approach of coupling membrane separation and heterogeneous photocatalytic technologies for the successful abatement of pharmaceutical compounds in effluents of wastewater treatment plants.
Hierarchical ZSM-5 zeolites synthesized by silanization of protozeolitic units: mediating the mesoporosity contribution by changing the organosilane type
(Elsevier, 2014) Serrano, D. P.; Pinnavaia, T. J.; Aguado, J.; Escola, J. M.; Peral, A.; Villalba, L.
Hierarchical ZSM-5 zeolites were prepared by crystallization of silanized protozeolitic units employing silylated polypropylene oxide diamine polymers as organosilanes. The influence of the (Sipol/ Sigel) molar ratio was investigated within 0 - 0.15 range. High synthesis yields (~90%) of well-crystallized hierarchical zeolites exhibiting a high proportion of secondary porosity (additional to the zeolitic micropores) was reached for (Sipol/Sigel) molar ratios lower than 0.08. The usage of the silylated polymer resulted in hierarchical ZSM-5 with larger mesopores (4-20 nm) in higher share than the hierarchical ZSM-5 prepared with a smaller organosilane (phenyl-aminopropyl-trimethoxysilane, PHAPTMS). However, it also contained meaningfully lower amount of acid sites and with less acid strength. The best catalytic performance in the cracking of low density polyethylene (LDPE) was showed by the material prepared from a (Sipol/Sigel) ratio of 0.03. Noteworthy, in addition to the gasoline range fraction (C6-C12), light C1-C5 olefins are the main reaction products, which are interesting feedstock for the petrochemical industry. Its catalytic performance is similar to the hierarchical ZSM-5 prepared using the smaller organosilane (PHAPTMS), which is indicative that the enhanced accessibility to the acid sites due to the presence of larger mesopores (4-20 nm) makes up for the lower amount and strength of its acid sites. Thereby, it is possible to enhance the mesoporosity by using bulkier organosilane (silylated polymers) but at the expense of losing acid properties.
SYNTHESIS OF HIERARCHICAL ZSM-5 BY SILANIZATION AND ALKOXYLATION OF PROTOZEOLITIC UNITS
(ELSEVIER, 2011) Serrano, D.P.; Aguado, J.; Escola, J.M.; Peral, Ángel; Morales, Gabriel; Abella, E.
Hierarchical ZSM-5 zeolite has been synthesized by means of a method involving a precrystallization stage to form the protozeolitic units, the addition and subsequent grafting of both silanization and alkoxylation agents, and a final hydrothermal crystallization. The influence of the alkoxylation with different alcohols (methanol, ethanol, 2-propanol and n-butanol) on the properties of the final hierarchical ZSM-5 samples has been investigated. In every case, the alcohol addition increased the incorporation of the seed silanization agent as it decreases the gel viscosity. In addition, the presence of alcohols deeply affects the physicochemical properties of the final materials. The samples prepared with 2-propanol and methanol were highly crystalline and presented improved textural properties with regard to the reference h-ZSM-5 and n-ZSM-5. In contrast, the samples obtained with ethanol and n-butanol were partially and totally X-ray amorphous, respectively. 1H and 13C-CP solid state MAS NMR spectra proved the alkoxylation of the external surface of the protozeolitic units. Catalytic cracking of LDPE pointed out the higher TOF values obtained over the hierarchical samples prepared with methanol and 2-propanol due to a right combination of accessibility and crystallinity in these materials. The differences observed among the samples prepared with alcohols were ascribed to the strong interaction produced between the silanization agent and the linear alcohols on the surface of the protozeolitic nanounits, which form a very stable protective layer, hindering their aggregation and subsequent crystallization.