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| 2. |
- Thormählen, Peter, 1969, et al.
(författare)
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The Influence of CO2, C3H6, NO, H2, H2O or SO2 on the Low-Temperature Oxidation of CO on a Cobalt-Aluminate Spinel Catalyst (Co1.66Al1.34O4)
- 2001
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Ingår i: Applied Catalysis B: Environmental. - 0926-3373 .- 1873-3883. ; 31:1, s. 1-12
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Tidskriftsartikel (refereegranskat)abstract
- A preparation method for making a high temperature stable monolith catalyst, using a cobalt-rich cobalt-aluminate spinel (Co1.66Al1.34O4) as the active material, is proposed. This catalyst, which is known for being active for CO oxidation at low temperatures, was prepared and characterised by BET, SEM, XRD, XPS and CO-TPD. The catalyst was tested for its capacity to oxidise carbon monoxide using oxygen only and oxygen in combination with other compounds typically present in cold start exhausts from Otto engines, i.e. CO2, C3H6. NO, H2, H2O or SO2. When the catalytic activity was tested with only CO and O-2 present in the feed gas, complete conversion was reached at room temperature. When other compounds were present in the gas mixture, they inhibited the CO oxidation to various degrees. The degree of inhibition for the compounds investigated was found to be: SO2 > H2O > NO = C3H6 > H2 > CO2. The main reason for the loss of activity is suggested to origin from the compounds adsorption and formation of different species on the cobalt oxide surface, which seems to inhibit the reduction and/or re-oxidation process of the metal oxide surface and/or the adsorption of CO.
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| 3. |
- Carlsson, Per-Anders, 1972, et al.
(författare)
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A transient in situ FTIR and XANES study of CO oxidation over Pt/Al2O3 catalysts
- 2004
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Ingår i: Journal of Catalysis. - : Elsevier BV. - 0021-9517 .- 1090-2694. ; 226:2, s. 422-434
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Tidskriftsartikel (refereegranskat)abstract
- We report experimental results for the oxidation of CO over supported Pt/Al2O3 catalysts operating in oxygen excess at atmospheric pressure. To study the reaction kinetics under transient conditions we have employed step changes of the O2 concentration by intermittently switching off the O2 supply at various temperatures ranging from 523 to 623 K. Detailed in situ FTIR and XANES data for CO coverage and the chemical state of Pt, respectively, are presented together with the CO conversion, which in both cases was monitored by mass spectrometry. A red-shift of the vibrational frequency of linearly bonded CO which correlates with a blue-shift of the Pt LIII binding energy indicates that the Pt catalyst initially is partially oxidised and gradually reduced when the O2 supply is switched off. Control experiments with a NO2 oxidised Pt/Al2O3 catalyst support these findings. A hysteresis in the catalytic activity due to the different rates whereby Pt is oxidised and reduced as a function of gas-phase composition is observed. The activation energy for the Pt oxide reduction (decomposition) process is estimated to be about 50 kJ/mol. The results further emphasise that the conventional three-step Langmuir-Hinshelwood (LH) scheme used to interpret CO oxidation on Pt surfaces must be complemented by a Pt oxidation and reduction mechanism during transient conditions. Moreover, FTIR data suggest that during the extinction, the partially oxidised platinum surface is reduced by chemisorbed CO which should be explicitly accounted for in the modeling of the reaction mechanism.
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| 8. |
- Carlsson, Per-Anders, 1972, et al.
(författare)
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Low-temperature CO oxidation over a Pt/Al2O3 monolith catalyst investigated by step-response experiments and simulations
- 2004
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Ingår i: Topics in Catalysis. - 1572-9028 .- 1022-5528. ; 30/31:1-4, s. 375-381
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Tidskriftsartikel (refereegranskat)abstract
- The ignitionextinction processes for CO oxidation over a Pt/Al2O3 monolith catalyst have been studied by flow-reactor experiments and simulations. The study was performed by stepwise changes of the inlet O2 concentration ranging 020 vol% while the CO concentration and the inlet gas temperature were kept constant at 1.0 vol% and 423 K, respectively. Several features observed experimentally are qualitatively simulated with our model: (i) the ignition of the CO oxidation demands 8.0vol% O2 (ii) corresponding to a catalyst ignition temperature of 433 K (due to the exothermicity of the reaction) and (iii) occurs in the rear part of the monolith where (iv) a local reaction zone is formed which (v) moves towards the reactor inlet as a function of time on stream. Additionally, the simulations show first order kinetic phase transitions, i.e. rapid adsorbate concentration changes, where the catalyst surface is predominantly CO covered in the low reactive state and almost completely oxygen covered in the high reactive state. For the ignition process the kinetic phase transition occurs after the actual catalytic ignition. However, the extinction process is more difficult to simulate dynamically without changing the model parameters for O2 adsorption in the low and high reactive state, respectively. The influence of diffusion limitations and the role of formation of a less reactive Pt state under oxidising conditions is discussed.
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| 10. |
- Carlsson, Per-Anders, 1972, et al.
(författare)
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Periodic control for improved low-temperature catalytic activity
- 2001
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Ingår i: Topics in Catalysis. - 1572-9028 .- 1022-5528. ; 16-17:1-4, s. 343-347
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Tidskriftsartikel (refereegranskat)abstract
- The influence of transient changes in the gas composition on the low-temperature activity of a commercial three-way catalyst and a Pt/Al2O3 model catalyst has been studied. By introducing well-controlled periodic O2 pulses to simple gas mixtures of CO or C3H6 (in N2), a substantial improvement of the low temperature oxidation activity was observed for both catalysts. The reason for low activity at low temperatures is normally attributed to self-poisoning by CO or hydrocarbons. The improved catalytic performance observed here is suggested to origin from the transients causing a surface reactant composition that is favourable for the reaction rate.
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