| 1. |
- Abdulhamid, Hussam, 1974, et al.
(författare)
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A combined transient in situ FTIR and flow reactor study of NOx storage and reduction over M/BaCO3/Al2O3 (M=Pt, Pd or Rh) catalysts
- 2006
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Ingår i: Journal of Catalysis. - : Elsevier BV. - 0021-9517 .- 1090-2694. ; 244:2, s. 169-182
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Tidskriftsartikel (refereegranskat)abstract
- Transient in situ DRIFTS and flow-reactor experiments were performed to study the storage and reduction of NOX over Pt/BaCO3/Al2O3, Pd/BaCO3/Al2O3, and Rh/BaCO3/Al2O3 samples using CO, H-2, C3H6, or C3H8 as the reducing agent. The DRIFTS results show that exposure of the examined samples to NO2 results in the formation of nitrite/nitrate peaks over alumina and barium and that the reduction of stored NOX is influenced by the type of precious metal and reducing agent. Using CO as the reductant results in a lower NOX reduction capacity for Pt/BaCO3/Al2O3 compared with Pd- and Rh-based samples, whereas H-2 shows a significant ability to reduce the stored NOX on all samples examined. In addition, the reduction with CO and C3H6 proceeds via the formation of isocyanate species over both barium and alumina sites. The intensity of barium-isocyanate species for Pt/BaCO3/Al2O3 is significantly lower than the corresponding intensity for the Pd- and Rh-based samples, suggesting that the interaction between barium and Pt is lower than the corresponding interaction in the Pd/BaCO3/Al2O3 and Rh/BaCO3/Al2O3 samples. (c) 2006 Elsevier Inc. All rights reserved.
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| 2. |
- Abdulhamid, Hussam, 1974, et al.
(författare)
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In situ FTIR study of SO2 interaction with Pt/BaCO3/Al2O3 NOx storage catalysts under lean and rich conditions
- 2006
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Ingår i: Journal of Catalysis. - : Elsevier BV. - 0021-9517 .- 1090-2694. ; 241:1, s. 200-210
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Tidskriftsartikel (refereegranskat)abstract
- The interaction of SO2 with Pt/BaCO3/Al2O3 NOx storage catalysts under lean and rich conditions in the absence and presence of water was investigated by means of in situ FTIR spectroscopy at 350 degrees C. For the lean condition (SO2 + O-2), surface and bulk barium sulfates were formed in addition to sulfites and surface sulfates on alumina. Pt does not appear to play an essential role in the formation of these species under lean conditions. In contrast, under reducing conditions (SO2 + H-2), Pt catalysed the reduction of SO2 with H-2 to form reduced sulfur species that accumulate on both Pt and barium sites. A subsequent treatment with NO2 resulted in the reduction of NO2 in the oxidation of these sulfur-containing species to form bulk barium sulfate instead of being stored over barium sites. Introducing water significantly affected sulfur trapping over the catalyst surface. During the lean conditions, the presence of water resulted in almost no surface barium sulfate formation. Meanwhile, the formation of bulk barium sulfate was increased, probably due to enhanced sulfate formation. However, the presence of H2O under reducing conditions resulted in significantly lower sulfur storage on both barium and alumina in comparison with humid lean exposure conditions.
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| 3. |
- Acke, Filip, 1968, et al.
(författare)
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Selective reduction of NO by HNCO over Pt promoted Al2O3
- 1998
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Ingår i: Journal of Catalysis. - : Elsevier BV. - 0021-9517 .- 1090-2694. ; 179:2, s. 528-536
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Tidskriftsartikel (refereegranskat)abstract
- The activity of Pt supported on gamma-Al2O3 towards HNCO oxidation and reduction of NO by HNCO under oxygen excess is examined under transient conditions (temperature ramps between 100 and 500 degrees C). Formation of N-2, N2O, NO, and NO2 is observed. Isotope labelled (NO)-N-15 is used to show the scrambling of nitrogens in N-2 ((NN)-N-14-N-15) and N2O ((NNO)-N-14-N-15). Adsorbed species on the surface are characterised by in-situ FTIR spectroscopy in order to obtain information on reaction intermediates. Adsorbed NNx species are discussed as important intermediates in the N-2 and N2O formation. The absence of Pt results in a delay in HNCO ignition and only a small N2O formation is observed.
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| 4. |
- Agrell, J., et al.
(författare)
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Production of hydrogen from methanol over Cu/ZnO catalysts promoted by ZrO2 and Al2O3
- 2003
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Ingår i: Journal of Catalysis. - : Elsevier BV. - 0021-9517 .- 1090-2694. ; 219:2, s. 389-403
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Tidskriftsartikel (refereegranskat)abstract
- Production of H-2 from methanol by steam reforming, partial oxidation, or a combination thereof was studied over Cu/ZnO-based catalysts. The catalysts were characterized by a variety of techniques, including N2O chemisorption, X-ray photoelectron spectroscopy, X-ray diffraction, and temperature-programmed reduction/oxidation. The influence of feed composition, reaction temperature, and catalyst formulation on H-2 production rate, product distribution, and catalyst lifetime was investigated. Distinct differences between the processes were observed with respect to catalyst behavior. ZrO2-containing catalysts, especially Cu/ZnO/ZrO2/Al2O3, exhibit the best performance in the steam reforming reaction. During partial oxidation, however, a binary Cu/ZnO catalyst exhibits the lowest light-off temperature and the lowest level of CO by-product. The redox properties of the catalyst appear to play a key role in determining the pathway for H-2 production. In particular. the extent of methanol and/or H-2 combustion at differential O-2 conversion is strongly dependent on the ease of copper oxidation in the catalyst.
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| 5. |
- Amandusson, H., et al.
(författare)
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Isotopic study of ethanol dehydrogenation over a palladium membrane
- 2000
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Ingår i: Journal of Catalysis. - : Elsevier BV. - 0021-9517 .- 1090-2694. ; 195:2, s. 376-382
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Tidskriftsartikel (refereegranskat)abstract
- The dehydrogenation of ethanol and the subsequent permeation were studied on a Pd membrane in a continuous ethanol supply. Hydrogen could not be extracted as efficiently from ethanol as from methanol. In ethanol, at least four of the six hydrogen atoms were not available for permeation because of methane formation. Hydrogens bonded to a carbon atom in a C-O group were available for permeation, while hydrogen atoms bonded to a carbon atom without oxygen were not. The efficiency of hydrogen permeation from ethanol was 5% compared to that of pure hydrogen, which could be compared to 25% for methanol compared to pure hydrogen. The hydrogen permeation could be enhanced by adding CO to the EtOH + O2 supply. The permeation probability of the hydrogen bonded to the methylene hydrogen increased while the water formation with this hydrogen atom decreased. Acetic acid was formed upstream when oxygen was in excess. The differently bonded hydrogen atoms in an ethanol molecule experienced different reaction pathways. The results did not contradict the models made from surface experiments in ultrahigh vacuum by Davis and Barteau, Holroyd and Bowker, or Bowker et al.
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| 6. |
- Amberntsson, Annika, 1974, et al.
(författare)
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Sulphur deactivation of NOx storage catalysts; Influence exposure conditions and noble metal
- 2003
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Ingår i: Journal of Catalysis. - 0021-9517 .- 1090-2694. ; 217:2, s. 253-263
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Tidskriftsartikel (refereegranskat)abstract
- In the present study, barium-based NOx, storage catalysts containing platinum, rhodium, or both noble metals were investigated. The influence of SO2 exposure conditions on the performance of NOx storage catalysts was studied using flow reactor measurements, FTIR, and XPS where the samples were exposed to lean and/or rich SO2-containing gas mixtures, simulating the conditions in a mixed lean application. The main results show that all samples are sensitive to sulfur and that deactivation is faster when SO2 is present in the feed under rich conditions than under lean or continuous SO2 exposure. It was also found that SO2 affects the performance of noble metals strongly and that noble metal deactivation most likely occurs during the rich period of a NOx storage cycle. Additionally, the influence of the noble metals present in the catalysts was investigated with respect to sulfur sensitivity and it was found that a combination of platinum and rhodium seems to be preferable for retaining high performance (high NO oxidation and reduction activity) of the catalyst under SO2 exposure and subsequent regeneration.
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| 7. |
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| 8. |
- Andersson, Arne, et al.
(författare)
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Activities of V-Ti-O Catalysts in the Ammoxidation of 3-Picoline
- 1980
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Ingår i: Journal of Catalysis. - : Elsevier BV. - 1090-2694 .- 0021-9517. ; 65:1, s. 9-15
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Tidskriftsartikel (refereegranskat)abstract
- Ammoxidation of 3-picoline was studied on reduced V-Ti-O catalysts with V6O13 as the major vanadium oxide. The results showed that the initial activity as a function of the TiO2 content reached a maximum at 50–60 mole% TiO2. It is proposed that there is maximum contact between the vanadium and titanium phases at this composition, which results in a weakening of the (VO)3+ surface bond. The selectivity of formation of nicotinonitrile exhibited a maximum of 83% at 10 mole% TiO2 and minima of 73 and 75% at 0 and 30 mole% TiO2, respectively. At higher TiO2 concentrations the selectivity increased continuously to 83% at 90 mole% TiO2. The variation of the selectivity of formation of nicotinonitrile depends on the View the MathML source ratio in the TiO2 phase. It was also found that the conversion and yields varied with the reaction time, which could be explained by the fact that reduced vanadium oxides were oxidized to V2O5 during the ammoxidation process. This oxidation leads to the formation of active and highly selective boundary surfaces between the TiO2-promoted vanadium oxides V6O13 and V2O5.
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| 9. |
- Andersson, Arne
(författare)
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Activities of V-Ti-O Catalysts in the Ammoxidation of 3-Picoline. II. Acid-Base Properties and Infrared Spectra
- 1982
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Ingår i: Journal of Catalysis. - : Elsevier BV. - 1090-2694 .- 0021-9517. ; 76:1, s. 144-156
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Tidskriftsartikel (refereegranskat)abstract
- The acidity and basicity of prereduced V-Ti-O catalysts were measured by adsorption of NH3 and CO2. It was found that a high activity in the ammoxidation of 3-picoline corresponds to a relatively small amount of acidic sites. A catalyst selective in the formation of nicotinonitrile requires high concentrations of both acidic and basic sites. These results are discussed, and can be correlated if the acidity is considered to be a measure of the hydroxyl group concentration, and the basicity a measure of oxygen vacancies in the vicinity of VO groups. Also, the infrared spectra of the prereduced catalysts were recorded. A new band was found at 995 cm−1. The same band appeared in a homogeneous mixture of V2O5 and V6O13. It is proposed that this band can be assigned to VO bonds in a reduced V2O5phase with a number of disordered vacancies in the lattice, or a nonstoichiometric V6O13 phase. The shift in frequency relative to that of (VO)3+ shows that these bonds are weaker, and probably also more active. The effect of TiO2 is to increase the amount of V4+ in the vanadium oxide lattice. This is caused by dissolution of Ti4+ in the V2O5 melt during the catalyst preparation.
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| 10. |
- Andersson, Arne, et al.
(författare)
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Activities of Vanadium Oxides in Ammoxidation of 3-Picoline
- 1979
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Ingår i: Journal of Catalysis. - 1090-2694. ; 58:3, s. 383-395
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Tidskriftsartikel (refereegranskat)abstract
- Ammoxidation of 3-picoline to nicotinonitrile was studied on V2O5, V6O13, and V2O4 catalysts in a fixed-bed integral reactor. The activity studies showed that V6O13 was the most active and selective catalyst of the pure oxides, with a maximum yield of 76% nicotinonitrile at 365 °C. The maximum yield on V2O5 catalyst was 34%, and was obtained at a higher temperature, 458 °C. V2O4 was found to be inactive under the conditions studied. The activities and selectivities of the oxides changed rapidly with reaction time when V6O13 and V2O4 were studied. By means of X-ray diffraction and a titrimetric method, the average oxidation number of vanadium was determined, V6O13 was both oxidized and reduced during the reaction; V2O4 was oxidized, while a relatively smaller reduction of V2O5 could be detected. The experiments showed that the V6O13 catalyst used, with both V2O5 and V6O13 phases present, was more selective than any of the pure oxides. This may be explained by active boundary surfaces. Also a mechanism of formation of nicotinonitrile is proposed, which includes a step in which an adsorbed aldehyde complex reacts with ammonia.
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