RESUMEN
We report for the first time the selective hydrogenation of 1,3-butadiene to butene using formic acid as the hydrogen source with 1 wt% Pd/carbon in a continuous flow reactor. The catalytic results show that the selectivity is even higher when formic acid is used compared to gas hydrogen.
RESUMEN
Au nanoparticles of different sizes were supported by the deposition-precipitation method on two metal oxides: ZnO and TiO2. The resulting catalysts were tested in the ethanol catalytic transformation reaction. Both metal oxide support materials exerted a different influence on the achieved Au particle size as well as on the behavior of the subsequent catalyst, with regard to their initial conversion values, product distribution and stability. While TiO2 favors the formation of smaller nanoparticles, ZnO offers larger Au particle sizes when prepared under similar conditions. At the same time, TiO2 produced catalysts which displayed higher initial conversions in comparison with AuZnO catalysts, even when observing catalysts of each series with similar particle sizes. At the same time, catalysts supported on ZnO exhibited higher resistance to deactivation caused by coke formation. These results were evidenced employing different characterization techniques on both used and fresh catalyst samples. The decline in deactivation was generally accompanied by an increase in the carbon content on the catalyst's surface.
RESUMEN
Hollow nanospheres of molybdenum disulfide have been synthesized by a novel solvothermal method under low temperature (180 degrees C). These nanomaterials were characterized by X-ray diffraction (XRD), Fourier transformation infra-red spectroscopy (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM, HRTEM) and X-ray Photoelectron Spectroscopy (XPS). A mechanism for the synthesis reaction is tentatively proposed and discussed.
RESUMEN
The Temporal Analysis of Products (TAP) technique has been used to investigate the mechanism involved in the catalytic decomposition of NH(3) over a series of catalysts consisting of activated carbon supported Ru (promoted and non-promoted with Na) and over an activated carbon supported Ir. An extensive study of the role played by both the support and the promoter in the "side reactions" and in the stability and surface lifetime of the NH(x) species has been performed. It was suggested that the N(2) produced during the first steps of the reaction over the activated carbon supported Ru catalysts promoted with Na forms a Na-N-Ru complex at the promoter-transition metal crystallite interface. This study also suggests that the Na promoter prevents the diffusion of hydrogen from the metal to the support via spill-over. A similar effect was observed after the thermal treatment at high temperature of the carbon catalyst support. Finally large differences in multi-pulse TAP results have been detected between Ru and Ir catalysts implying that the NH(3) decomposition reaction mechanism must be different on both metals.
RESUMEN
Two graphitic carbon materials with different edge to basal plane ratio, high surface area graphite (HSAG) and graphitized carbon nanofibers (CNFs), were oxidized by two methods, aqueous-HNO(3) wet oxidation and oxygen plasma oxidation. Characterization of the materials by temperature-programmed desorption, thermogravimetry and X-ray photoelectron and Raman spectroscopies indicated that the amount and nature of oxygen surface groups introduced depended on the oxidation method and on the structure of the original material. While surface sites within the layers were only oxidized by oxygen plasma, surface sites at the edges of graphene layers were oxidized by both treatments being the wet oxidation more effective. Modification of the oxidized materials with a diamine or a triamine molecule resulted in the formation of ammonium carboxylate salt species on the carbon surface.
RESUMEN
The adsorption from aqueous solutions of a series of non-ionic surfactants (TX-114, TX-100, TX-165 and TX-305, where the ethoxylation degree is increasing in the series) on a non-microporous carbon surface, that is a high surface area graphite (GT), and on a mainly microporous activated carbon (NT) has been comparatively studied. Also the initially hydrophobic GT and NT surfaces have been modified by oxidation treatments in order to achieve partially hydrophilic carbon materials (GTox and NTox samples). The adsorption results reveal that for GT sample below the critical micellar concentrations (cmc) of surfactants practically the whole surface is covered by monomers. For NT there are steric hindrance limitations, so the surfactant molecules are adsorbed only on micropores of sizes larger than 8A. When oxygen surface groups are introduced on the carbonaceous surfaces, the adsorption behaviour is again different for both materials. Thus, for GTox the adsorbed amounts below the cmc decrease probably due to withdrawal effect of the oxygen surface groups. On the contrary, the adsorbed amounts above the cmc slightly increase with regard to bare graphite, possibly due to an improved formation of micelles. In the case of NTox the adsorbed uptakes below and above cmc increase remarkably in comparison with NT sample, which can be explained by some specific interactions of the surfactants molecules with oxygen surface groups inside the micropores.
RESUMEN
57Fe Mössbauer spectroscopy was used to study the reduction behavior at temperatures as high as 1073 K of an iron/silica catalyst, and also the carbonaceous materials isolated after acetylene decomposition over this catalyst at several temperatures (873-1073 K). The products were previously characterized by transmission electron microscopy and it was clearly proven that the concentration of carbon nanotubes increased when reaction reached highest temperatures. This was related with an increment in cementite concentration (generated from initial alpha-iron and the progressive reduction of the remnant Fe+2 caused by acetylene decomposition) as detected by 57Fe Mössbauer. These results undoubtedly revealed the role of alpha-iron as active center for acetylene decomposition and cementite as main carbide intermediate species in the catalytic growth of CNTs.
RESUMEN
Adsorption of phenol and nonylphenol from aqueous solutions on microporous activated carbons has been studied. The phenol isotherm changes from L-shaped for surface oxygen group free carbon (I sample) to a two-stepped isotherm for oxidized carbon (IN sample, HNO(3) treated) Furthermore, the adsorbed amounts diminish in about 25% on IN carbon. It is proposed that a change in the adsorption mechanism take place; i.e., weak interaction forces between the pi electrons in phenol and the pi electron in carbon are present on the original I carbon, while a donor-acceptor complex on the oxidized IN carbon is operating between basic surface oxygen groups and phenol aromatic rings. The shape of nonylphenol isotherms is two-stepped for both carbons. The introduction of acidic oxygen surface groups on the carbon enhances the specific nonylphenol adsorption by about 40%. This may be interpreted as being due to the fact that nonylphenol is hydrogen-bonded to the oxidized carbon surface by means of acidic groups. Thermal desorption experiments indicate that phenol is mainly physisorbed. Thermal desorption further confirms that nonylphenol is possibly bonded to oxygen surface groups by hydrogen bonds. Copyright 2001 Academic Press.
RESUMEN
The adsorption processes of two different types of surfactant from aqueous solutions have been studied on several solids. The adsorbates used were a nonionic (TX-100) and a series of anionic (NP4S, NP10S, and NP25S) oxyethylenic surfactants. As adsorbent, five nonporous solids, including three quartz (QA, QB, and QC), a kaolin, and a dolomite, were chosen for this study, since these types of materials are frequently found in oil reservoirs. Great differences have been found in the adsorption plateaus, depending on the nature of the surfactant (anionic or nonionic). The influence of the presence of NaCl and CaCl2 in the solutions has been also studied. NaCl affects the adsorption of anionic surfactants on quartz and kaolin samples in a similar way. When this salt is added, the amount of anionic surfactants adsorbed on the solid surfaces increases. Some differences in the adsorption of the TX-100 surfactant, depending on the nature of the surface and the type of salt added, have been detected. Basically, three different adsorption behaviors have been found when NaCl is added. The amounts of TX-100 adsorbed decrease when NaCl is added to the solution on the QA sample; the amounts increase on the QB and kaolin samples; no alteration is observed on QC and dolomite samples. Changes in adsorption isotherms, depending on whether NaCl or CaCl2 is added, have also been observed. For the same five adsorbents, zeta potential measurements also have been carried out. When the nonionic TX-100 surfactant is adsorbed, a decrease in the negative values of the zeta potential takes place. However, for the adsorption of anionic surfactants, an increase in the negative values of the zeta potential is detected. The surface charge has been also determined by potentiometric titration (in presence and in absence of TX-100), and a decrease in surface charge when TX-100 is adsorbed on the sample surfaces has been detected. Copyright 1998 Academic Press.