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Sökning: L773:0920 5861 OR L773:1873 4308

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1.
  • Hammarstrom, L., et al. (författare)
  • Mimicking photosystem II reactions in artificial photosynthesis : Ru(II)-polypyridine photosensitisers linked to tyrosine and manganese electron donors
  • 2000
  • Ingår i: Catalysis Today. - 0920-5861 .- 1873-4308. ; 58:03-feb, s. 57-69
  • Tidskriftsartikel (refereegranskat)abstract
    • The paper describes a project aiming at constructing functional mimics of the oxygen evolving complex in photosystem II, coupled to photoinduced charge separation. Biomimetic electron donors, manganese complexes and tyrosine, have been linked to a Ru(II)-polypyridine photosensitiser. Oxidation of the donors by intramolecular electron transfer from the photooxidised Ru(III) complex was demonstrated using optical flash photolysis and EPR experiments. A step-wise electron transfer Mn(III,III)-->tyrosine-->Ru(III) was demonstrated, in analogy to the reaction on the donor side of photosystem II. Electron transfer from the tyrosine to Ru(III) was coupled to tyrosine deprotonation. This resulted in a large reorganisation energy and thus a slow reaction rate, unless the tyrosine was hydrogen bonded or already deprotonated. A comparison with analogous reaction in photosystem II is made. Finally, light-induced oxidation of a manganese dimer linked to a Ru(II)-photosensitiser was observed. Preliminary results suggest the possibility of photooxidising manganese dimers in several steps, which is an important step towards water oxidation,
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2.
  • Berg, M., et al. (författare)
  • Catalytic combustion of low heating value gas mixtures : comparison between laboratory and pilot scale tests
  • 2000
  • Ingår i: Catalysis Today. - 0920-5861 .- 1873-4308. ; 59:02-jan, s. 117-130
  • Tidskriftsartikel (refereegranskat)abstract
    • Catalytic combustion of low heating value fuels is a promising method for electricity production combining the use of a renewable fuel with ultra-low emissions. In the present work, catalytic combustion of a low heating value gas has been studied over monolithic catalysts in an atmospheric 30 kW pilot catalytic combustor connected to a wood pellet gasifier. The results have been compared to similar tests with a model gas mixture and a series of test in a laboratory scale reactor for monolithic samples. Various catalyst configurations have been tested, such as precious metal-based catalyst impregnated on modified alumina washcoats and hexaaluminate washcoats. Cordierite monoliths with various cells per square inch were used as supports, but hexaaluminate extruded monoliths were also used. The catalysts were combined in different segment series. The results show that it is possible to ignite the low heating value gas at compressor outlet temperatures without the use of pre-burners over precious metal catalysts. Generally, trends and phenomena obtained in laboratory reactor operating close to isothermal could be confirmed in the pilot operating at close to adiabatic conditions. Further results, such as deactivation by sulphur compounds, fuel-NOx conversion and emissions of carbon monoxide and total hydrocarbons, are addressed in the paper.
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3.
  • Ersson, A., et al. (författare)
  • Catalytic combustion of methane over bimetallic catalysts a comparison between a novel annular reactor and a high-pressure reactor
  • 2003
  • Ingår i: Catalysis Today. - 0920-5861 .- 1873-4308. ; 83:04-jan, s. 265-277
  • Tidskriftsartikel (refereegranskat)abstract
    • The effects of adding a co-metal, Pt or Rh, to Pd/-gamma-Al2O3 catalysts were studied with respect to the catalytic activity for methane combustion and compared to a Pd/gamma-Al2O3 catalyst, using both a pressurized pilot-scale and a lab-scale annular reactor. Temperature programmed oxidation (TPO) experiments were also carried out to investigate the oxygen release/uptake of the catalyst materials. Palladium showed an unstable behavior both in the pilot and lab-scale experiments at temperatures well below the PdO to Pd transformation. An addition of Pt to Pd stabilized, and in some cases increased, the catalytic activity for methane combustion. The TPO experiments showed that the oxygen release peak was shifted to lower temperatures even for low additions of Pt, i.e. Pd:Pt = 2:1. For additions of rhodium only small beneficial effects were seen. The steady-state behavior of the lab-scale annular reactor correspond well to the pressurized pilot-scale tests.
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4.
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5.
  • Lassinantti, Magdalena, et al. (författare)
  • Preparation and evaluation of thin ZSM-5 membranes synthesized in the absence of organic template molecules
  • 2001
  • Ingår i: Catalysis Today. - 0920-5861 .- 1873-4308. ; 67:1-3, s. 109-119
  • Tidskriftsartikel (refereegranskat)abstract
    • Porous α-alumina supports with a pore size of 100 nm were seeded with colloidal TPA-silicalite-1 crystals with a size of 120 nm. The seeded supports were calcined and treated in a synthesis solution free from organic template molecules to form ZSM-5 films on the supports. According to SEM images, the films were about 2 μm thick and no defects could be found on the as-synthesized membranes. Single gas permeation data was collected and good quality membranes (defined as having a non-detectable permeance of SF6 after drying at 100°C) were further evaluated using binary/ternary gas mixtures. The selectivity for n-butane/i-butane had a maximum value of 17.8 at 220°C. Water was selectively separated from a helium-diluted vaporized water/ethanol azeotrope with a maximum selectivity of 12.4.
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6.
  • Pocoroba, E., et al. (författare)
  • Ageing of palladium, platinum and manganese-based combustion catalysts for biogas applications
  • 2000
  • Ingår i: Catalysis Today. - 0920-5861 .- 1873-4308. ; 59:02-jan, s. 179-189
  • Tidskriftsartikel (refereegranskat)abstract
    • During recent years, catalytic combustion of low heating value gases has received increased attention. The purpose of the present work was to study the effect of ageing for 30 days at 1000 degrees C in air saturated with 12% steam on Pd- and Pt-impregnated as well as Mn-substituted lanthanum hexaaluminate materials. Both hexaaluminate powders and 400 cpsi cordierite monoliths, washcoated with hexaaluminate powder, were aged. Powders were characterised by BET and XRD, whereas the catalytic activity of the washcoated monoliths was evaluated in a bench-scale rig for conversion of synthetic gasified biomass. The surface areas decreased significantly during the first day of ageing, whereas further ageing had only a minor influence. The pure lanthanum-alumina sample was a mixture of the hexaaluminate LaAl11O18 phase and the less preferable perovskite LaAlO3 phase, which increased after ageing. The Mn-substituted lanthanum-alumina mainly showed pure hexaaluminate phase both before and after ageing. The catalytic activity tests showed that Pd-impregnated lanthanum hexaaluminate was the most active catalyst for combustion of carbon monoxide and hydrogen, retaining low light-off temperatures also after 30 days of ageing. However, the ignition temperature for 50% conversion (T-50) of methane was approximately 300 degrees C higher than for the fresh sample. Pt-impregnated samples were less active than the Pd ones. The Pt-loading decreased after ageing, whereas the Pd-loading remained fairly constant. However, the amount of Pd oxide decreased after ageing. Further, the Mn-substituted samples were less active than the precious metal ones. Here, the activity for the combustion of carbon monoxide was substantially affected by ageing. The formation of nitrogen oxides from ammonia was lower over the aged samples than over fresh ones; the Mn-substituted sample aged 30 days showed the lowest yield, only 30% of ammonia was converted to nitrogen oxides.
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7.
  • Pradier, C.M., et al. (författare)
  • NO reduction by isobutene, in the presence of oxygen, on platinum and copper : a comparative study
  • 1996
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 29:1-4, s. 59-65
  • Tidskriftsartikel (refereegranskat)abstract
    • The reaction of NO, oxygen and isobutene was studied under conditions close to stoichiometric, on a platinum and on a copper disk in order to better understand the role of each metal, free of any support and dispersion effects. The products of the reaction were analysed by mass spectrometry and an XPS characterization of the surface was carried out at different stages of the reaction. A correlation between the catalytic activity for NO conversion and the presence of adsorbed intermediates has been clearly demonstrated on platinum. On copper, a redox cycle of the metal is necessary to activate the catalyst. On platinum, oxygen is necessary to initiate the reaction, clean the surface and form reactive intermediates; the reaction is strongly sensitive to oxygen concentration, whereas on copper, oxygen does not directly participate in the reaction mechanism.
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8.
  • Rymes, J., et al. (författare)
  • Microemulsions in the preparation of highly active combustion catalysts
  • 2002
  • Ingår i: Catalysis Today. - 0920-5861 .- 1873-4308. ; 75:1-4, s. 297-303
  • Konferensbidrag (refereegranskat)abstract
    • Catalytic activity in combustion of toluene in toluene-air mixtures and physical-chemical properties of platinum catalysts prepared from reverse microemulsions (water-in-oil) and by classical impregnation from water solutions of H2PtCl6 were studied. Microemulsion catalysts were more active than those prepared classically from water solutions. Size of Pt in classically impregnated catalysts was three times higher than that of catalysts prepared from microemulsions. In case of microemulsion preparation method, platinum is located near the pellet surface or its position in the pellet can be optimised. The effect of oil used in microemulsion system seems to be negligible for the activity of the catalysts with 0.1 wt.% Pt.
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9.
  • Sterte, Johan, et al. (författare)
  • Application of the seed-film method for the preparation of structured molecular sieve catalysts
  • 2001
  • Ingår i: Catalysis Today. - 0920-5861 .- 1873-4308. ; 69:1-4, s. 323-329
  • Tidskriftsartikel (refereegranskat)abstract
    • The seed-film method has been applied for the preparation of various materials of potential interest as structured molecular sieve catalysts. The method has proven to be very flexible and allows for the reproducible preparation of a number of molecular sieve–substrate combinations as well as the control of the materials’ properties of importance in catalytic applications such as zeolite loading, film thickness, film density and crystal orientation. The preparation of thin molecular sieve films on ceramic foams, α-alumina pellets and porous alumina supports as well as various metal surfaces is described. The preparation of zoned coatings with a compositional gradient is also discussed.
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10.
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11.
  • Ahmadi, Mozhgan, et al. (författare)
  • Development of an on-line tar measurement method based on photo ionization technique
  • 2011
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 176:1, s. 250-252
  • Tidskriftsartikel (refereegranskat)abstract
    • This paper presents work in progress for development of an on-line method based on PID (Photo Ionization Detector) for quantitative measurement of tar from biomass gasification. To calibrate the method the PID signals are compared to quantitative data of individual tar compounds obtained by an established reference method. The measured response factors for the model tar compounds demonstrated very good linearity. The PID approach was tested on-line with real producer gases from an atmospheric fluidized bed gasifier operated at 800-900 °C. The results suggest that PID can be used for continuous on-line tar measurement of product gases from biomass gasification.
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12.
  • Albertazzi, S, et al. (författare)
  • The technical feasibility of biomass gasification for hydrogen production
  • 2005
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 106:1-4, s. 297-300
  • Tidskriftsartikel (refereegranskat)abstract
    • Biomass gasification for energy or hydrogen production is a field in continuous evolution, due to the fact that biomass is a renewable and CO2 neutral source. The ability to produce biomass-derived vehicle fuel on a large scale will help to reduce greenhouse gas and pollution, increase the security of European energy supplies, and enhance the use of renewable energy. The Varnamo, Biomass Gassification Centre in Sweden is a unique plant and an important site for the development of innovative technologies for biomass transformation. At the moment, the Varnamo plant is the heart of the CHRISGAS European project, that aims to convert the produced gas for further upgrading to liquid fuels as dimethyl ether (DME), methanol or Fischer-Tropsch (F-T) derived diesel. The present work is an attempt to highlight the conditions for the reforming unit and the problems related to working with streams having high contents of sulphur and alkali metals.
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13.
  • Barrientos, Javier, et al. (författare)
  • Further insights into the effect of sulfur on the activity and selectivity of cobalt-based Fischer–Tropsch catalysts
  • 2016
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 275, s. 119-126
  • Tidskriftsartikel (refereegranskat)abstract
    •  A sulfur poisoning study was performed by ex situ poisoning of a platinum-promoted cobalt/alumina catalyst with different sulfur amounts. The poisoned catalyst samples were tested at relevant Fischer–Tropsch reaction conditions and at the same CO conversion in order to evaluate the effect of sulfur on catalyst activity and product selectivity. It was found that the activity and the selectivity to long-chain hydrocarbons decrease with increasing sulfur content. Moreover, it was found that sulfur has no significant effect on the CO2 selectivity. It was also shown that sulfur significantly enhances olefin hydrogenation. Finally, a deactivation model relating the catalyst activity and the sulfur to cobalt active site ratio was proposed and used to describe the experimental results.
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14.
  • Bernardini, A., et al. (författare)
  • Direct synthesis of H2O2 over Pd supported on rare earths promoted zirconia
  • 2015
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 256, s. 294-301
  • Tidskriftsartikel (refereegranskat)abstract
    • In this work Pd (0.3 or 0.6 wt.%) was supported on both ZrxM1-xO2 (M = La, Y, Ce) and on mechanical mixtures of CeO2 and ZrO2. The synthesized catalysts were characterized by XRD, TPR, AAS and CO chemisorption and tested for the direct synthesis of hydrogen peroxide in a high pressure semibatch apparatus. The reactants conversion was limited in order to avoid mass-transfer limitations. No selectivity enhancers of any kind were used and the all the materials were halide free. Small metal particles were obtained (1-2.6 nm). Supports with smaller pore diameters leaded to larger Pd particles, which in turn were found to preferentially support the formation of the peroxide. Moreover, supports with higher reducibility favored the production of H2O2, probably due to an easier reduction of the active metal, essential to achieve high selectivity. Notwithstanding the absence of enhancers, the specific activity and selectivity recorded were very high.
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15.
  • Biasi, Pierdomenico, et al. (författare)
  • Application of the Catalyst Wet Pretreatment Method (CWPM) for catalytic direct synthesis of H2O2
  • 2015
  • Ingår i: Catalysis Today. - : Elsevier. - 0920-5861 .- 1873-4308. ; 246:Special Issue, s. 207-215
  • Tidskriftsartikel (refereegranskat)abstract
    • This work concerns a new technique to post-modify the catalytic material intended for use in H2O2 direct synthesis. The catalyst chosen was a commercially available 1 wt.% Pd/C. The catalyst was modified with the so-called Catalyst Wet Pretreatment Method (CWPM) that is used to post-modify prepared catalysts with aqueous solutions of NaBr, in different concentrations. The performance of pristine and the pretreated materials were then compared in the H2O2 direct synthesis and characterized before and after the catalytic tests in order to understand the role of the different concentrations of bromide in the CWPM procedure. The surface features of the different catalysts were analyzed with CO chemisorption (metal dispersion and mean particle size), Transmission Electron Microscopy (TEM, for Pd morphology and Pd particle size distributions), Inductive Coupled Plasma (ICP, for Pd content) and Ion Chromatography (IC, for bromide content). Various features of the materials prepared with the CWPM were correlated with the catalytic performance. It was found that the bromide has an active role in the reconstruction of metal phase and it does not only act as a poison for the most active catalytic sites as often reported in literature. By using this new protocol, the production H2O2 was almost doubled compared to the non-modified material when no direct promoters were added to the reaction environment.
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16.
  • Bora, Tanujjal, et al. (författare)
  • Defect engineered visible light active ZnO nanorods for photocatalytic treatment of water
  • 2017
  • Ingår i: Catalysis Today. - : ELSEVIER SCIENCE BV. - 0920-5861 .- 1873-4308. ; 284, s. 11-18
  • Tidskriftsartikel (refereegranskat)abstract
    • Photocatalytic degradation of organic wastes and microbes in water using solar light is a green technology that requires the design of visible light active photocatalysts. Here we report the fabrication of visible light active zinc oxide nanorods (ZnO NRs), wherein the visible light absorption is enhanced by modulating the surface defects on the NRs. Oxygen vacancies in the NRs as characterized by photoluminescence and X-ray photoelectron spectroscopy are controlled by annealing at different temperatures in the ambient. The role of surface defects on the visible light photocatalytic degradation of an organic dye, industrial waste, bacterial culture and inland brackish water is studied. Results presented here provide a simple strategy to make the wide bandgap ZnO NRs visible light active, enabling their use for the photocatalytic decontamination of water.
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17.
  • Boutonnet, Magali, et al. (författare)
  • Microemulsion droplets to catalytically active nanoparticles : How the application of colloidal tools in catalysis aims to well designed and efficient catalysts
  • 2017
  • Ingår i: Catalysis Today. - : Elsevier. - 0920-5861 .- 1873-4308. ; 285, s. 89-103
  • Tidskriftsartikel (refereegranskat)abstract
    • In this review, we report the successful application of a colloidal tool, namely microemulsions (ME) in the design of catalysts for various applications. First, a brief introduction to MEs and the water-in-oil (w/o) ME reaction method is given. The first ME formulations used for catalyst synthesis are discussed. Catalytic activity of the materials obtained from those initial studies, both as particles deposited onto a support as well as directly as nanoparticles in ME suspension is described. Then various application examples which highlight several important properties of the catalysts obtained from w/o ME are given. For example, particle size control achieved with ME is very relevant to surface sensitive reactions, whose selectivity depends greatly on metal particle size. Another important aspect is related to the unique microenvironment of MEs which results in specific interactions within the formed materials; this is particularly important for certain catalysts such as mixed oxide particles, conferring them with special properties and enhanced performance. Comparison of activity and selectivity of impregnation-prepared versus ME-prepared materials is given for several catalytic reactions. Finally, the more recently developed oil-in-water (o/w) ME method is described, along with examples of materials obtained by this method as catalysts, including photocatalysis. The different aspects discussed in this review demonstrate the importance of the ME reaction method for the design of nanocatalysts with enhanced activity and selectivity.
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18.
  • Busch, Michael, 1983, et al. (författare)
  • Validation of binuclear descriptor for mixed transition metal oxide supported electrocatalytic water oxidation
  • 2013
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 202:1, s. 114-119
  • Tidskriftsartikel (refereegranskat)abstract
    • The energy profiles of the di-hydroxo – di-oxo – peroxo pathway are discussed for a set of 3d transition metal oxides comprising V(III–V), Cr(III–V), Mn(II–IV, Mn(III–V), Fe(II–IV), Co(II–IV) and Ni(II–IV) using density functional theory (DFT). Two classes of oxides were identified. The first class, comprising V(III–V), Cr(III–V) and Fe(II–IV), displays exothermicity for the oxidation of di-hydroxo to di-oxo versus the tyrosine/tyrosyl-radical (TyrOH/TyrO) couple and endothermicity for the subsequent O-O bond formation ([−/+] class), while the second class, comprising Mn(III–V), Co(II–IV) and Ni(II–IV), shows endothermicity with respect to the oxidation step and exothermicity for the O-O bond formation ([+/−] class). The energetics of the endothermicity (exothermicity) for the oxidation step is reflected in the exothermicity (endothermicity) of the subsequent O-O bond formation step. Mn(II–IV) is not part of any of the two classes. Instead it shows zero exothermicity with respect to TyrOH/TyrO for the oxidation step and a small endothermicity for the O-O bond formation step. Despite the promising energy profile Mn(II–IV) is argued to be inactive due to a large activation barrier. A set of improved hetero-nuclear candidate catalysts is predicted by mixing [−/+] with [+/−] transition metal oxides. A simple and efficient method to estimate the energy profile of mixed transition metal oxides from the homo-nuclear systems is demonstrated. The validity of this procedure is checked and agreement with the explicitly calculated values is found. All considered heteronuclear candidate catalysts display enhanced performance compared to the pure homonuclear systems.
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19.
  • Dahlin, Sandra, et al. (författare)
  • Chemical aging of Cu-SSZ-13 SCR catalysts for heavy-duty vehicles –Influence of sulfur dioxide
  • 2018
  • Ingår i: Catalysis Today. - Amsterdam : Elsevier. - 0920-5861 .- 1873-4308. ; 320, s. 72-83
  • Tidskriftsartikel (refereegranskat)abstract
    • Selective catalytic reduction of nitrogen oxides is an efficient technique for emission abatement in heavy-dutyvehicles. Cu-SSZ-13 SCR catalysts are more active than vanadium-based catalysts at low temperatures, but aremore sensitive to deactivation by sulfur. Consequently, there is a need to study poisoning by sulfur for thiscatalyst material. This experimental investigation focuses on the effect of sulfur on the low-temperature per-formance of Cu-SSZ-13 SCR catalysts. The effect of sulfur exposure temperature, and the influence of the NO 2 /NO x ratio, are considered and two different regeneration temperatures are compared. In addition, catalystsamples from an engine-aged catalyst are evaluated. The SO 2 exposure temperature is shown to have an im-portant impact on the deactivation of the Cu-SSZ-13 catalyst. The lowest sulfur exposure temperature (220 °C)results in the most severe deactivation, while the highest temperature during sulfur exposure (400 °C) results inthe lowest degree of deactivation. This was found to be related to the amount of sulfur on the catalyst.Additionally, SO 2 exposure was shown to decrease the N 2 O selectivity. The engine-aged catalyst has a decreasedperformance in terms of both decreased activity and increased N 2 O selectivity. For this catalyst, impurities fromfuel and engine-oil can play a role in the deactivation. Different deactivation mechanisms are seen for the lab-and engine-aged catalysts.
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20.
  • Dahlin, Sandra, et al. (författare)
  • Effect of biofuel- and lube oil-originated sulfur and phosphorus on the performance of Cu-SSZ-13 and V2O5-WO3/TiO2 SCR catalysts
  • 2021
  • Ingår i: Catalysis Today. - : Elsevier B.V.. - 0920-5861 .- 1873-4308. ; 360, s. 326-339
  • Tidskriftsartikel (refereegranskat)abstract
    • Two different SCR catalysts, V2O5-WO3/TiO2 and Cu-SSZ-13, were exposed to biodiesel exhausts generated by a diesel burner. The effect of phosphorus and sulfur on the SCR performance of these catalysts was investigated by doping the fuel with P-, S-, or P + S-containing compounds. Elemental analyses showed that both catalysts captured phosphorus while only Cu-SSZ-13 captured sulfur. High molar P/V ratios, up to almost 3, were observed for V2O5-WO3/TiO2, while the highest P/Cu ratios observed were slightly above 1 for the Cu-SSZ-13 catalyst. Although the V2O5-WO3/TiO2 catalyst captured more P than did the Cu-SSZ-13 catalyst, a higher degree of deactivation was observed for the latter, especially at low temperatures. For both catalysts, phosphorus exposure resulted in suppression of the SCR performance over the entire temperature range. Sulfur exposure, on the other hand, resulted in deactivation of the Cu-SSZ-13 catalyst mainly at temperatures below 300-350 °C. The use of an oxidation catalyst upstream of the SCR catalyst during the exhaust-exposure protects the SCR catalyst from phosphorus poisoning by capturing phosphorus. The results in this work will improve the understanding of chemical deactivation of SCR catalysts and aid in developing durable aftertreatment systems. 
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21.
  • Das, T., et al. (författare)
  • Charge transfer driven interaction of CH4, CO2 and NH3 with TiS2 monolayer : Influence of vacancy defect
  • 2021
  • Ingår i: Catalysis Today. - : Elsevier B.V.. - 0920-5861 .- 1873-4308. ; 370, s. 189-195
  • Tidskriftsartikel (refereegranskat)abstract
    • In this work we have investigated the dissociation of hydrogen rich CH4 and NH3 molecules along with CO2 on the surface of pristine and various defect induced TiS2 monolayer. The aim is to see whether the monolayer surfaces are able to produce H2 by decomposing the feedstock adsorbates and also to examine whether it can be a sorbent for CO2. We have tried to explore a monolayer surface which can simultaneously act as a catalyst to dissociate CH4, as well as to adsorb CO2 which is the only harmful by-product in steam reforming method for hydrogen production from CH4. The hydrogen generation has been predicted from the nature of gas adsorption, and the adsorption energies have been estimated to see whether it falls under chemisorption or physisorption range. Both S and Ti vacancy defects have been studied and the first-principles electronic structure calculation helps to envisage the charge redistribution of the three adsorbates on both pristine and defective TiS2 surfaces.
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22.
  • Elm Svensson, Erik, et al. (författare)
  • Microemulsion synthesis of MgO-supported LaMnO3 for catalytic combustion of methane
  • 2006
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 117:4, s. 484-490
  • Tidskriftsartikel (refereegranskat)abstract
    • Catalysts with 20% LaMnO3 supported on MgO have been prepared via CTAB-1-butanol-iso-octane-nitrate salt microemulsion. The preparation method was successfully varied in order to obtain different degrees of interaction between LaMnO3 and MgO as shown by TPR and activity tests after calcination at 900 degrees C. Activity was tested on structured catalysts with 1.5% CH4 in air as test gas giving a GHSV of 100,000 h(-1). The activity was greatly enhanced by supporting LaMnO3 on MgO compared with the bulk LaMnO3. After calcination at 1100 degrees C both the surface area and TPR profiles were similar, indicating that the preparation method is of little importance at this high temperature due to interaction between the phases. Pure LaMmO(3) and MgO were prepared using the same microemulsion method for comparison purposes. Pure MgO showed an impressive thermal stability with a BET surface area exceeding 30 m(2)/g after calcination at 1300 degrees C. The method used to prepare pure LaMnO3 appeared not to be suitable since the surface area dropped to 1.1 m(2)/g already after calcination in 900 degrees C.
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23.
  • Eriksson, Sara, et al. (författare)
  • Fuel-rich catalytic combustion of methane in zero emissions power generation processes
  • 2006
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 117:4, s. 447-453
  • Tidskriftsartikel (refereegranskat)abstract
    • A novel catalytic combustion concept for zero emissions power generation has been investigated. Catalysts consisting of Rh supported on ZrO2, Ce-ZrO2 or alpha-Al2O3 were prepared and tested under fuel-rich conditions, i.e. for catalytic partial oxidation (CPO) of methane. The experiments were performed in a subscale gas-turbine reactor operating at 5 bar with exhaust gas-diluted feed mixtures.The catalyst support material was found to influence the light-off temperature significantly, which increased in the following order Rh/Ce-ZrO2 < Rh/ZrO2 < Rh/alpha-Al2O3. The Rh loading, however, only had a minor influence. The high activity of Rh/Ce-ZrO2 is probably related to the high dispersion of Rh on Ce-ZrO2 and the high oxygen mobility of this support compared to pure ZrO2. The formation of hydrogen was also found to increase over the catalyst containing ceria in the support material.
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24.
  • Eriksson, Sara, et al. (författare)
  • Partial oxidation of methane over rhodium catalysts for power generation applications
  • 2005
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 100, s. 447-451
  • Tidskriftsartikel (refereegranskat)abstract
    • The partial oxidation of methane (POM) to syngas, i.e. H-2 and CO, over supported Rh catalysts was investigated at atmospheric pressure. The influence of support material, Rh loading and the presence of water vapor on the methane conversion efficiency and the product gas composition was studied. The catalysts containing ceria in the support material showed the highest activity and formation of H2 and CO. By increasing the Rh loading, a decrease of the ignition temperature was obtained. The addition of water vapor to the reactant gas mixture was found to increase the ignition temperature and the formation of hydrogen, which is favorable for combustion applications where the catalytic POM stage is followed by H-2-stabilized homogeneous combustion.
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25.
  • Ersson, Anders, et al. (författare)
  • A comparison between hexaaluminates and perovskites for catalytic combustion applications
  • 2006
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 112:04-jan, s. 157-160
  • Tidskriftsartikel (refereegranskat)abstract
    • Hexaaluminates and perovskites are two promising candidates for use in catalytic combustion applications. In the present study two hexaaluminates, LaMnAl11O19 and LaCoAl11O19, were compared with two perovskites, LaMnO3 and LaCoO3, with respect to their thermal stability and catalytic activity for combustion of methane and gasified biomass. The results showed that the hexaaluminates retained a much higher surface area even after calcination at 1200 degrees C compared to the perovskites. LaMnAl11O19 showed the highest catalytic activity of all catalysts. LaCoAl11O19 generally showed low activity. Of the two perovskites, LaCoO3 was the most active, and the initial test run the activity for biomass combustion were close to that one of LaMnAl11O19 even though its surface area was only one tenth of the hexaaluminate's. However, it was severely deactivated in the second test run. Similar deactivation but less severe was also found for the other catalyst.
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26.
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27.
  • Gonzalez, Angelica V., et al. (författare)
  • Full-scale autothermal reforming for transport applications : The effect of diesel fuel quality
  • 2013
  • Ingår i: Catalysis Today. - : Elsevier. - 0920-5861 .- 1873-4308. ; 210, s. 19-25
  • Tidskriftsartikel (refereegranskat)abstract
    • This study evaluates the feasibility of H-2 production through a fuel flexible reformer, at realistic operating conditions for electricity supply by FC-APUs in the transport sector. The fuel flexibility is evaluated by comparison of autothermal reforming performance with biodiesel (RME), Fischer-Tropsch, low-sulfur diesel (MK1) and European standard diesel (DIN 590). ATR experiments with two monolithic catalysts, Rh1.0Pt1.0Ce10La10/Al2O3 (CAT 1) and Rh1.0Pt1.0Mg4.0Y5.0/CeO2-ZrO2 (CAT 2), sequentially placed in the axial direction of the reformer length were used for full-scale tests. The O-2/C ratio was varied from 0.3 to 0.5 and the H2O/C ratio varied from 2 to 3.5, reaching temperatures in the interval of 700-800 degrees C. The hydrogen production and fuel conversion showed an upward trend from RME < DIN 590 < MK1 < FT with maximum 42 vol.% H-2 and 99% fuel conversion for FT diesel.
  •  
28.
  • Grahn, Mattias, et al. (författare)
  • Small ZSM-5 crystals with low defect density as an effective catalyst for conversion of methanol to hydrocarbons
  • 2020
  • Ingår i: Catalysis Today. - : Elsevier B.V.. - 0920-5861 .- 1873-4308. ; 345, s. 136-146
  • Tidskriftsartikel (refereegranskat)abstract
    • This work presents the synthesis of nearly defect-free ZSM-5 nanosized crystals, prepared in fluoride medium by seeding with silicalite-1. This material was carefully characterized and its catalytic performances in the methanol to hydrocarbons (MTH) reaction were assessed. Such fluoride-based material was compared to a reference ZSM-5, produced through a conventional alkaline synthesis but from the same seeding. Despite both the materials show closely identical morphology and they have a comparable acid site population, the catalyst prepared using the fluoride route showed significantly longer lifetime in MTH compared to the catalyst prepared using conventional synthesis at high pH. The slower deactivation for the samples prepared using the fluoride route was ascribed, thanks to a thorough in situ IR spectroscopy study, to its lower density of internal defects. According to the UV-Raman characterization of coke on the spent catalyst, the fluoride-based ZSM-5 catalyst produces less molecular coke species, most probably because of the absence of enlarged cavities/channels as due to the presence of internal defects. On the basis of these observations, the deactivation mechanism in the ZSM-5 synthesized by fluoride medium could be mostly related to the deposition of an external layer of bulk coke, whereas in the alkali-synthesized catalyst an additional effect from molecular coke accumulating within the porous network accelerates the deactivation process.
  •  
29.
  •  
30.
  • Huerta, I., et al. (författare)
  • Effect of low hydrogen to palladium molar ratios in the direct synthesis of H2O2 in water in a trickle bed reactor
  • 2015
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 248, s. 91-100
  • Tidskriftsartikel (refereegranskat)abstract
    • Application of a trickle bed reactor (TBR) renders a very compact solution to carry out direct synthesis of hydrogen peroxide in water over a carbon supported palladium. The laboratory scale reactor was filled with silica particles (50-70 mesh) physically mixed with 37.5 to 75 mg of 5%Pd/C particles. The reaction conditions applied were 15 degrees C, 15-28 barg, 0.5 to 6 mL min(-1) of liquid and 4.0-4.5 mL min(-1) of gas flowrate (86.7/11/2.23 mol% of CO2/O-2/H-2). Thus, we demonstrated that the ratio between H-2 and Pd is one of the key factors to achieve optimized, higher yields of hydrogen peroxide. Consequently, low H-2 concentrations lead to low productivities. One of the least studied parameters, addressed here, is the ratio between the bed filling (SiO2) and the catalyst; i.e. the active catalytic species dilution effect. In short, it was found that when the amount of Pd was reduced below 0.094 mg Pd cm(-3) SiO2 the highest productivity of H2O2 could be achieved. The selectivity obtained were between 5.3 and 38.0%, respectively, corresponding to turn-over-frequencies (TOF) ranging from 65 to 921 mmol H2O2 gPd(-1) h(-1). (C) 2014 Elsevier B.V. All rights reserved.
  •  
31.
  • Hyvärinena, S., et al. (författare)
  • Sugars and sugar derivatives in ionic liquid media obtained from lignocellulosic biomass : comparison of capillary electrophoresis and chromatographic analysis
  • 2014
  • Ingår i: Catalysis Today. - : Elsevier. - 0920-5861 .- 1873-4308. ; 223, s. 18-24
  • Tidskriftsartikel (refereegranskat)abstract
    • Processing of woody lignocellulosic biomass, under heating in combination with ionic liquids (ILs) was studied in order to obtain simple (fermentable) sugars. Due to the new environmental challenges, finding greener ways to produce platform chemicals and/or bio-fuels has become a popular research area. Various industrial, pilot or laboratory scale technologies for the depolymerization or fractionation of lignocellulosic polysaccharides to monomers are known. One of the new, interesting, methods is to utilize ILs in biomass pre-treatment procedures with an aim to bypass other pre-treatment methods. Furthermore, in order even to initiate studies whether ILs can contribute to catalytic depolymerization, there has to be a robust way to analyze the IL-treated lignocellulosics. This is a major issue since woody samples that contain any salts such as ILs can indeed be quite challenging from the analytic point of view. The applied capillary electrophoresis was found to be an excellent analytical method providing substantial improvements compared to the earlier used chromatographic methods.In this work it was demonstrated that application of ILs, at elevated temperatures, contributes to hydrolysis and depolymerization of lignocellulose. The effect is time and temperature dependent: in harsh conditions sugars degrade but too low processing temperatures or short treatment times result in no meaningful effect. The formation of the degradation products of the monosaccharides is a good indicator of the harshness of the applied chemical conditions. Evidently, furfural and 5-(hydroxymethyl)furfural formed in rather short treatment times.
  •  
32.
  • Karatzas, Xanthias, et al. (författare)
  • Hydrogen generation from n-tetradecane, low-sulfur and Fischer-Tropsch diesel over Rh supported on alumina doped with ceria/lanthana
  • 2011
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 164:1, s. 190-197
  • Tidskriftsartikel (refereegranskat)abstract
    • The present study demonstrates the use of rhodium-based monolithic catalyst for onboard reforming of diesel fuels. Experimental results from hydrogen generation of n-tetradecane, low-sulfur and Fischer-Tropsch diesel, via autothermal reforming (ATR), were acquired with a catalyst consisting of 3 wt% Rh supported on alumina doped with Ce/La. The catalyst was prepared by impregnation using the incipient wetness technique, and deposited onto a 400 cpsi cordierite monolith. Furthermore, the catalyst was tested over ranges of oxygen-to-carbon and water-to-carbon feed ratios, both in a bench-scale and a full-scale reactor. Fresh powder samples of the catalyst were characterized by XRD, N(2)-BET, H(2) chemisorption, H(2)-TPR and XPS analyses. The activity results showed that high fuel conversions and hydrogen production could be achieved with 3 wt% Rh for all fuels. Furthermore, the highest formation of CO and C(2)H(4) was found in the product gas stream from the low-sulfur diesel. In addition, partial oxidation and steam reforming reactions were identified by closely studying the distribution of the analyzed product gas composition and the temperature measurements. The characterization results showed the presence of finely dispersed Rh particles in the support. Furthermore, bulk and surface rhodium oxides were detected, which have been suggested to be one of the major active phases for ATR of diesel. Bulk and surface cerium oxides (CeO(2)) and surface La in the dispersed phase were also found to be present in the catalyst composition. These promoters are believed to improve the catalyst activity and durability.
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33.
  • Karatzas, Xanthias, et al. (författare)
  • Microemulsion and incipient wetness prepared Rh-based catalyst for diesel reforming
  • 2011
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 175:1, s. 515-523
  • Tidskriftsartikel (refereegranskat)abstract
    • The role of the catalyst preparation technique was investigated for diesel reforming. Reverse microemulsion (ME) and incipient wetness (IW) techniques were used for the preparation of Rh-based monolithic catalysts that were employed for hydrogen generation of low-sulfur diesel via autothermal reforming (ATR). The washcoat of the tested catalysts consisted of 0.5 wt% Rh, 1 wt% Rh, and 1: 1 wt% Rh: Pt supported on gamma-alumina. All washcoats were deposited on 400 cpsi cordierite monoliths. The reaction condition was T(feed) = 650 degrees C, H(2)O/C similar to 2.5, O(2)/C similar to 0.49, TOS = 3 h, GHSV similar to 13 000 h(-1) and P = 1 atm. Fresh and aged powder samples of the catalyst were characterized by N(2)-BET, H(2) chemisorption, XRD, H(2)-TPR, O(2)-TPO and TEM. The activity results established that Rh and RhPt formulations, prepared by ME and IW, are highly active for ATR of diesel where fuel conversions above 92% were obtained. FTIR and NDIR analysis also showed that the highest formation of ethylene was found in the product gas stream from the bimetallic samples indicating that RhPt/Al(2)O(3) is less resistant towards carbon deposition. The latter observation was confirmed by O(2)-TPO analysis of the aged samples where high loads of coke were found both on the active metals and on the support. Interestingly, these effects were less significant on the ME samples. The characterization results clearly showed differences in morphology between the ME and the IW samples. N(2)-BET analysis showed that higher surface area, similar to 268-285 m(2)/g, was obtained with the ME samples. Also, H(2) chemisorption analysis showed that the rhodium dispersion was similar to 10% higher for the ME samples (H/Rh similar to 60-66%). XRD analysis showed that crystalline phases of gamma-alumina were present on all samples. The diffractograms also showed small traces of metallic Pt (similar to 16-30 nm) in the bimetallic samples. H(2)-TPR analysis, showed peaks ascribed to bulk rhodium oxides and rhodium aluminates. It was also noted that the addition of Pt on the support lowered the reducibility of the different rhodium species. TEM analysis performed on the fresh and aged ME and IW bimetallic samples showed mainly Rh(x)Pt(1-x) alloys with an average particle size of similar to 20-50 nm were present on the alumina support. Also, for the aged samples, no sintering effects were noted. Furthermore, rhodium was found to switch oxidation state from e. g. Rh(3+) to Rh(0) while Pt remained in the metallic state.
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34.
  • Kirilin, Alexey V., et al. (författare)
  • Aqueous phase reforming of xylitol over Pt-Re bimetallic catalyst : Effect of the Re addition
  • 2014
  • Ingår i: Catalysis Today. - : Elsevier. - 0920-5861 .- 1873-4308. ; 223, s. 97-107
  • Tidskriftsartikel (refereegranskat)abstract
    • The aqueous phase reforming (APR) of xylitol was studied in a continuous fixed bed reactor over three catalysts: Pt/Al2O3, Pt/TiO2 and Pt-Re/TiO2. The data obtained in the case of the monometallic Pt catalysts was compared to the bimetallic Pt-Re sample. The effect of Re addition on the catalyst stability, activity, product formation and selectivity toward hydrogen and alkanes was studied. The bimetallic catalyst demonstrated a higher selectivity to alkanes compared to the monometallic samples. The monometallic catalyst was more selective toward hydrogen formation. A plausible reaction scheme explaining differences in selectivity toward hydrogen and alkanes was proposed and discussed.
  •  
35.
  • Laguna, O. H., et al. (författare)
  • Au-supported on Fe-doped ceria solids prepared in water-in-oil microemulsions : Catalysts for CO oxidation
  • 2016
  • Ingår i: Catalysis Today. - : Elsevier. - 0920-5861 .- 1873-4308. ; 278, s. 140-149
  • Tidskriftsartikel (refereegranskat)abstract
    • Gold catalysts were synthesized by deposition-precipitation employing Fe-doped ceria systems, previously obtained by means of the water-in-oil microemulsions methodology with different iron contents (10, 25 and 50 Fe at.%). The final catalysts were tested in the CO oxidation reaction in presence of H-2. After gold deposition the crystalline structure of the supports was not altered. Moreover no XRD lines associated to gold were detected, indicating its high dispersion. Solid solution was generated in all samples, although the segregation of iron oxide was detected for the material with the highest iron loading. This phenomenon was then enhanced for the corresponding gold catalyst that also presented sintering of the gold nanoparticles. Strong interaction between gold and the oxygen vacancies of the supports was demonstrated, as well as the promotion of the reducibility of surface Ce4+ and Fe3+ species at low temperatures. A remarkable promotion of the CO conversion at lower temperatures respect to that of the supports was observed for the gold catalysts. Below 120 degrees C, lower the amount of iron incorporated, higher the catalytic performance of the catalyst. This behaviour is closely related not only to a high gold dispersion but also to the ability for creating additional oxygen vacancies in the support, required for the CO oxidation reaction.
  •  
36.
  • Lanza, Roberto, et al. (författare)
  • NOx selective catalytic reduction over supported metallic catalysts
  • 2009
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 147, s. S279-S284
  • Tidskriftsartikel (refereegranskat)abstract
    • In this work we present the results obtained with 3 catalysts (Pt, Rh and Ag on alumina) tested in ranges of temperatures and gas hourly space velocities typical of diesel engines in real trucks. NO concentration was 500 ppm, C3H6 ranged between 500 and 2000 ppm, while oxygen was always 5%. All the catalysts were active and showed high conversions. Both Pt and Rh were active at low temperature (T-50 = 200-250 degrees C) but had quite high selectivity towards NO2. Silver was active at higher temperature, but showed very high selectivity towards N-2. A strong boosting effect on NO conversion was recorded if H-2 was added to the gas mixture.
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37.
  • Leino, Ewelina, et al. (författare)
  • Synthesis and characterization of ceria-supported catalysts for carbon dioxide transformation to diethyl carbonate
  • 2018
  • Ingår i: Catalysis Today. - : Elsevier. - 0920-5861 .- 1873-4308. ; 306, s. 128-137
  • Tidskriftsartikel (refereegranskat)abstract
    • The support materials Al2O3, SiO2 and TiO2 were modified with 16 wt% CeO2, using two different preparation methods evaporation-impregnation and precipitation-deposition. The synthesized 16 wt% CeO2-Al2O3, 16 wt% CeO2-SiO2 and 16 wt% CeO2-TiO2 materials were characterized by means of X-ray powder diffraction for the phase purity, scanning electron microscopy for the morphology, nitrogen physisorption to determine the specific surface area and X-ray photo electron spectroscopy for the oxidation state of the Ce in the TiO2, Al2O3 and SiO2 matrices. Transmission electron microscopy was used to study the particle size of CeO2 whereas CO2-temperature programmed desorption (TPD) was used to determine the basicity of ceria-modified TiO2, Al2O3 and SiO2 catalysts. Furthermore, the catalytic performance of the as prepared CeO2-modified catalysts were compared in the synthesis of diethyl carbonate starting from ethanol and CO2 using butylene oxide as the dehydrating agent. The physico-chemical characterization results were correlated with the catalytic activity results and discussed in detail.
  •  
38.
  • Leino, Ewelina, et al. (författare)
  • The influence of various synthesis methods on the catalytic activity of cerium oxide in one-pot synthesis of diethyl carbonate starting from CO2, ethanol and butylene oxide
  • 2013
  • Ingår i: Catalysis Today. - : Elsevier. - 0920-5861 .- 1873-4308. ; 210, s. 47-54
  • Tidskriftsartikel (refereegranskat)abstract
    • Different synthesis methods such as homogeneous precipitation at room temperature and supercritical water (T > 647 K and P > 22.1 MPa) were employed for cerium oxide preparation. Additionally, deposition of ceria on silica mesoporous material, SBA-15, was carried out. The obtained materials were characterized by means of X-ray powder diffraction, scanning electron microscopy, transmission electron microscopy, nitrogen physisorption, X-ray photoelectron spectroscopy and CO2 temperature programmed desorption. Considerable variations in physico-chemical properties of the resulting materials were observed. The catalytic activities of pristine cerium oxide and ceria loaded on SBA-15 support were compared. The test reaction was synthesis of diethyl carbonate starting from carbon dioxide and ethanol using butylene oxide as the dehydrating agent.
  •  
39.
  • Lualdi, Matteo, et al. (författare)
  • On the effect of water on the Fischer-Tropsch rate over a Co-based catalyst : The influence of the H2/CO ratio
  • 2013
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 214, s. 25-29
  • Tidskriftsartikel (refereegranskat)abstract
    • The effect of water partial pressure on the Fischer-Tropsch (FT) rate of a cobalt catalyst supported on narrow-pore γ-Al2O3 was investigated at industrially relevant process conditions (483 K, 30 bar, pellet size: 53-90 μm). Inlet water partial pressure was varied up to 9 bar by external water vapour addition at different H2/CO molar ratios ranging from 1 to 3. The effect of water was found to be positive on FT-rate independently of the H2/CO ratio, but more significantly at H 2-poor condition. Temperature-programmed hydrogenation (TPH) was used to verify the presence of unreactive carbon species on the catalyst after 22 h on stream at the different conditions with and without exposure to about 9 bar water. A higher temperature feature that could be associated to amorphous polymeric carbon was detected at H2-poor conditions but remained unchanged upon 2 h of water exposure which did not result in a change in the amount of amorphous polymeric carbon detectable by TPH.
  •  
40.
  • Montes, V., et al. (författare)
  • Chemoselective hydrogenation of furfural to furfuryl alcohol on ZrO2 systems synthesized through the microemulsion method
  • 2018
  • Ingår i: Catalysis Today. - : ELSEVIER SCIENCE BV. - 0920-5861 .- 1873-4308. ; 306, s. 89-95
  • Tidskriftsartikel (refereegranskat)abstract
    • Different solids consisting in hydrous zirconia were synthesized by the water in oil microemulsion technique (ME series). For comparative purposes, diverse solids were also obtained by the conventional sol-gel method (Pseries). The solids were tested for liquid-phase selective hydrogenation of furfural to furfuryl alcohol, using propan-2-ol as the hydrogen donor (Meerwein-Ponndorf-Verley process). The best results corresponded to catalysts calcined at 200 degrees C which consisted in amorphous solids with surface areas of ca 200 m(2)/g. The presence of some surfactant remaining from the synthetic process in solids obtained through the microemulsion technique favored selectivity to furfuryl alcohol with values >= 98%. Results were explained by the steric hindrance of furfural by the surfactant molecules in micelles thus favoring the interaction of the substrate with hydroxyl groups in hydrous zirconia through the C=O group. Application of microwave irradiation accelerated the reaction (15-30 times) as compared to conventional heating.
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41.
  • Montes, V., et al. (författare)
  • Preparation and characterization of Pt-modified Co-based catalysts through the microemulsion technique : Preliminary results on the Fischer-Tropsch synthesis
  • 2014
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 223, s. 66-75
  • Tidskriftsartikel (refereegranskat)abstract
    • The influence of the addition of small amounts of platinum (0.1-0.25% wt) to cobalt-based systems on Fischer-Tropsch synthesis was investigated. The solids were synthesized through microemulsion technique using TiO2 as the support. The best catalytic performance was achieved using Synperonic 13/6.5 as the surfactant. In all cases, the presence of platinum led to an increase in CO conversion which could be ascribed to the promotion of cobalt reducibility as evidenced by XPS. Moreover, the simultaneous reduction of cobalt and platinum precursors during synthetic procedure (ME1) was preferable to the consecutive one (ME2) probably as a result of a better Co-Pt interaction in the former case, as evidenced by TPR. TPR, Raman and XPS data also suggested that not only the presence of Co-0 but also the appearance of Co-TiO2 interactions favor the catalytic performance and that in general those interactions are stronger for ME1 solids.
  •  
42.
  • Montes, V., et al. (författare)
  • Selective transformation of glycerol into 1,2-propanediol on several Pt/ZnO solids : Further insight into the role and origin of catalyst acidity
  • 2015
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 257, s. 246-258
  • Tidskriftsartikel (refereegranskat)abstract
    • Microemulsion technique allowed us to synthesize different ZnO solids with similar particle sizes and textural properties. Platinum was subsequently incorporated by deposition-precipitation and impregnation methods and solids tested for glycerol selective transformation into 1,2-PDO. Incorporation of platinum led to the creation of new (mainly Lewis) acid sites. A good correlation between conversion and acidity of Pt/ZnO solids was obtained. Interestingly, despite exhibiting some acidity, supports alone were inactive in the process which evidenced the role of the metal in dehydration of glycerol into acetol. Furthermore, as the reaction proceeded some chlorine coming from the precursor (H2PtCl6) was leached which led to the disappearance of the strongest acid sites, associated to side reactions (catalytic cracking) thus resulting in an increase in selectivity to 1,2-PDO. Eventual formation of Pt-Zn alloy upon reduction of the systems at ca. 400 degrees C was beneficial to 1,2-PDO selectivity.
  •  
43.
  • Montes, V., et al. (författare)
  • Synthesis of different ZnO-supported metal systems through microemulsion technique and application to catalytic transformation of glycerol to acetol and 1,2-propanediol
  • 2014
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 223, s. 129-137
  • Tidskriftsartikel (refereegranskat)abstract
    • Different systems consisting of diverse metals (Au, Pt, Pd, Rh) supported on ZnO (5% by weight) were synthesized through the microemulsion technique (ME) and tested for glycerol hydrogenolysis, the main products being hydroxyacetone (acetol) and 1,2-propanediol (1,2-PDO). The solids synthesized using sodium borohydride as the reducing agent (B series) had smaller particle sizes as compared to the use of hydrazine (H series) which, in turn, resulted in a better catalytic performance. This synthetic method allowed us to obtain similar metal particle sizes (2-4 nm) for Pt, Pd and Rh solids in B series, whereas average gold metal particle was higher (> 8 nm) which probably accounts for Au-containing systems being inactive under our experimental conditions. Reactivity order followed the sequence Rh > Pt > Pd. A comparison of the systems synthesized in the present paper through ME technique with those obtained in a previous work through the deposition-precipitation process revealed a higher activity and selectivity to acetol for the former solids which could be related to the presence of surfactant. Moreover, results suggested that metal sites could participate not only in hydrogenation of acetol to 1,2-propanediol but also in the previous dehydration step of glycerol to acetol.
  •  
44.
  • Murzin, D. Yu., et al. (författare)
  • Arabinogalactan hydrolysis and hydrolytic hydrogenation usingfunctionalized carbon materials
  • 2015
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 257, s. 169-176
  • Tidskriftsartikel (refereegranskat)abstract
    • Hydrolysis of the hemicellulose arabinogalactan was studied in this work over several functionalized carbon materials, which were specifically treated to increase their acidities. Hydrolytic hydrogenation of arabinogalactan was investigated using the same materials in a mechanical mixture with ruthenium supported on active carbon. Application of these mixtures resulted in formation of polyols, suppressing simultaneously the generation of side products hydroxymethylfurfural (HMF) and furfural. Formation of high molecular weight compounds (aggregates of sugars and humins) was still quite substantial with a mechanical mixture of Ru/C and a carbon material prepared from sucrose by activation with zinc chloride to increase porosity. Post-treatment of this carbonaceous material with sulphuric acid significantly influenced kinetics of high molecular weight products formation resulting also in elevation of sugar alcohols yields.
  •  
45.
  • Nemanova, Vera, et al. (författare)
  • Biomass gasification in an atmospheric fluidised bed : Tar reduction with experimental iron-based granules from Höganäs AB, Sweden
  • 2011
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 176:1, s. 253-257
  • Tidskriftsartikel (refereegranskat)abstract
    • The present study investigates the effect of several experimental iron-based granules on biomass tar decomposition. The iron-based materials were provided by Höganäs AB and were all in their metallic state when they were applied in a secondary catalytic reactor. Bark-free birch was employed as fuel in an atmospheric fluidised bed reactor, and the tar concentration and gas composition in the producer gas were measured before and after the catalytic bed. The results demonstrate a clear tar reduction capacity for all the tested iron-based materials.
  •  
46.
  • Persson, Katarina, et al. (författare)
  • Supported palladium-platinum catalyst for methane combustion at high pressure
  • 2005
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 100, s. 479-483
  • Tidskriftsartikel (refereegranskat)abstract
    • Catalytic combustion of methane over a supported bimetallic Pd-Pt catalyst and a monometallic Pd catalyst has been investigated experimentally. Two different reactor configurations were used in the study, i.e. a tubular lab-scale reactor working at atmospheric pressure and a high-pressure reactor working at up to 15 bar. The results showed that the bimetallic catalyst has a clearly more stable activity during steady-state operation compare to the palladium only catalyst. The activity of the bimetallic catalyst was slightly higher than for the palladium catalyst. These results were established in both test facilities. Further, the impact of pressure on the combustion activity has been studied experimentally. The tests showed that the methane conversion decreases with increasing pressure. However, the impact of pressure is more prominent at lower pressures and levels out for pressures above 10 bar
  •  
47.
  • Regali, Francesco, 1971-, et al. (författare)
  • Effect of metal loading on activity, selectivity and deactivation behavior of Pd/silica-alumina catalysts in the hydroconversion of n-hexadecane
  • 2014
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 223, s. 87-96
  • Tidskriftsartikel (refereegranskat)abstract
    • Bifunctional catalysts consisting of palladium on amorphous silica-alumina with different metal loadings (0 wt% to 1.2 wt%) were compared in the hydrocracking/hydroisomerization of n-hexadecane. The reaction conditions were: pressure = 30 bar; temperature = 310 degrees C; hydrogen-to-hexadecane feed molar ratio = 10. Metal loading was found to have a remarkable influence on the initial deactivation rate, which could be related to the formation of carbonaceous deposits. The dependence of activity on the metal-acid site ratio was the typical one for bifunctional hydrocracking where, after reaching a threshold value, the catalytic activity does not appreciably increase with increasing metal loading. On the Pd-containing catalysts, the methane space-time-yield showed a strong dependence on conversion, but no clear relationship with metal surface area, indicating that the formation of methane might not proceed by purely metal-catalyzed hydrogenolysis.
  •  
48.
  • Regali, Francesco, et al. (författare)
  • Hydrocracking of n-hexadecane on noble metal/silica-alumina catalysts
  • 2013
  • Ingår i: Catalysis Today. - : Elsevier BV. - 0920-5861 .- 1873-4308. ; 214:SI, s. 12-18
  • Tidskriftsartikel (refereegranskat)abstract
    • Bifunctional catalysts consisting of platinum or palladium on amorphous silica-alumina were prepared and tested in the hydrocracking of n-hexadecane (n-C16H34). Product selectivities toward mono-branched and multi-branched feed isomers and cracking products have been determined in a wide range of conversions, varying liquid hourly space velocity at constant operating parameters (pressure = 30 bar; temperature = 310 C; H 2/n-C16H34 feed molar ratio = 10). A simple kinetic study is presented, in which the reactions are approximated by a network of pseudo first order irreversible reaction steps. The reaction network model was fitted to the experimental data, and kinetic constants for the different reaction steps were obtained. It could be concluded that mono-branched feed isomers are primary products in the hydrocracking/hydroisomerization reaction network; multi-branched isomers are formed mainly from mono-branched as a secondary product. On the platinum catalyst cracking products were formed as primary products, and it proved to be slightly more active than the palladium based one, at the same metallic molar loading. It could be shown that the platinum catalyst yields cracking products both via a bifunctional metal/acid mechanism and by monofunctional (metal only) hydrogenolysis. This second mechanism accounted for the higher activity of the platinum catalyst.
  •  
49.
  • Rytter, Erling, et al. (författare)
  • Hydrophobic catalyst support surfaces by silylation of gamma-alumina for Co/Re Fischer-Tropsch synthesis
  • 2018
  • Ingår i: Catalysis Today. - : Elsevier. - 0920-5861 .- 1873-4308. ; 299, s. 20-27
  • Tidskriftsartikel (refereegranskat)abstract
    • Eight different silanes with chloro or methoxy active ligands have been examined to modify the surface of a standard.-alumina support to investigate the effect of surface acidity and hydrophobicity in Fischer-Tropsch synthesis (FTS) at common operating conditions (210 degrees C; 20 bar; H-2/CO = 2.1). Silanes were impregnated prior to cobalt (Pre) or after cobalt impregnation and calcination (Post). Samples were characterized by standard techniques (FTIR, XRD, TPD, TPR, TGA, BET). In the Post series, cobalt crystallite size is maintained, while it is reduced when cobalt impregnation is performed on a partly hydrophobic surface. Both series of catalysts have FTS performances that deviate significantly from a reference catalyst and, in combination with characterization data, the silanes have modified all the 15 examined catalysts. The Pre series offer options for improved selectivity to higher hydrocarbons in FTS. The effects of silylation on FT performance mechanisms are discussed in terms of gas diffusion limitations, strain in cobalt particles and partial blocking of CO activation sites.
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50.
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Kumar, A. (4)
Fridell, Erik, 1963 (4)
Järås, Sven G. (4)
Hedlund, Jonas (4)
Salmi, Tapio (4)
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Brandin, Jan (4)
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Lundgren, Edvin (3)
Sá, Jacinto (3)
Akermark, B. (3)
Creaser, Derek, 1966 (3)
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Hansen, Staffan (3)
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Ahuja, Rajeev, 1965- (2)
Hammarstrom, L (2)
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Panas, Itai, 1959 (2)
Adams, Emma, 1989 (2)
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Zhang, Linus (2)
Jareman, Fredrik (2)
Persson, Katarina (2)
Virtanen, Pasi (2)
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Szabó, Péter (2)
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