| 1. |
- Wang, Xueting, 1991, et al.
(författare)
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Methanol Desorption From Cu-ZSM-5 Studied by In Situ Infrared Spectroscopy and First-Principles Calculations
- 2017
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 121:49, s. 27389-27398
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Tidskriftsartikel (refereegranskat)abstract
- The dynamic interaction of methanol and its derivatives with Cu-exchanged ZSM- 5 during methanol temperature programmed desorption from 30 to 450 ◦C has been investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy and first-principles calculations. The results emphasize that defects in the framework structure of the zeolite and Brønsted acid sites constitute ion-exchange sites for Cu ions. The Cu sites introduced in ZSM-5 actively interact with methanol adsorbed at moderate temperature, i.e. below 250◦C, and take roles in further oxidation of the adsorbed species to formate and CO. Moreover, spectra recorded at higher temperatures, i.e. above 300◦C, after adsorption of methanol show strong interaction between methoxy groups and the zeolite framework, suggesting that under mild conditions proton extraction for methanol production during direct partial oxidation of methane to methanol over Cu-ZSM-5 is necessary.
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| 2. |
- Dahlin, Sandra, et al.
(författare)
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Chemical aging of Cu-SSZ-13 SCR catalysts for heavy-duty vehicles –Influence of sulfur dioxide
- 2018
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Ingår i: Catalysis Today. - Amsterdam : Elsevier. - 0920-5861 .- 1873-4308. ; 320, s. 72-83
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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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| 3. |
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| 4. |
- Larsson, Ann-Charlotte, et al.
(författare)
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Pilot-scale investigation of Pt/alumina catalysts deactivation by organosilicon in the total oxidation of hydrocarbons
- 2007
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Ingår i: Topics in Catalysis. - : Springer Science and Business Media LLC. - 1572-9028 .- 1022-5528. ; 45:1-4, s. 121-124
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Tidskriftsartikel (refereegranskat)abstract
- The deactivation of alumina-supported platinum catalyst for VOC oxidation by long-term exposure for hexamethyldisiloxane (HMDS) has been investigated in a pilot scale reactor for up to 1000 h of exposure. Catalyst samples were characterized by ICP-AES, BET and silicon deposition by SEM. Catalyst activity was investigated using oxidation of ethyl acetate showing deactivation of the catalyst samples as exposed to HMDS increasing with exposure time. Silicon was shown to deposit on the catalyst as well as on the blank alumina support. SEM investigation of an individual pellet revealed a radial eggshell silicon distribution. CO chemisorption showed strong decrease of Pt active sites after deactivation, while still maintaining reasonable oxidation levels of ethyl acetate.
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| 5. |
- Martin, Natalia Mihaela, 1984, et al.
(författare)
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Characterization of Surface Structure and Oxidation/Reduction Behaviour of Pd-Pt/Al2O3 Model Catalysts
- 2016
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 120:49, s. 28009-28020
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Tidskriftsartikel (refereegranskat)abstract
- Structural and morphological characterisation of bimetallic Pd-Pt/Al2O3 model cat- alysts are performed using X-ray diffraction, X-ray absorption spectroscopy, transmis- sion electron microscopy and CO chemisorption. Further, the catalysts were studied under oxidising and reducing conditions using both X-ray absorption spectroscopy and low-energy ion scattering spectroscopy. For the as-prepared catalysts, the existence of alloyed bimetallic Pd-Pt particles and of (tetragonal) PdO were found for the samples calcined at 800 C. PdO is present in form of crystals at the surface of the Pd-Pt par- ticles or as isolated PdO crystals on the support oxide. Bimetallic Pd-Pt nanoparticles were only formed on the Pd-Pt catalysts after calcination at 800 C. The results show that the Pd-Pt nanoparticles undergo reversible changes in surface structure composi- tion and chemical state in response to oxidising or reducing conditions. Under oxidising conditions Pd segregates to the shell and oxidises forming PdO, while under reducing conditions regions with metallic Pd and Pd-Pt alloys were observed at the surface. No bimetallic Pd-Pt nanoparticles were observed for the sample initially calcined at 500 C, but instead isolated monometallic particles, where small Pt particles are easily oxidised under O2 treatment. In the monometallic catalysts, the Pd is found to be com- pletely oxidised already after calcination and to consist of metallic Pd after reductive treatment.
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| 6. |
- Martin, Natalia Mihaela, 1984, et al.
(författare)
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Structure-function relationship during CO2 methanation over Rh/Al2O3 and Rh/SiO2 catalysts at atmospheric pressure conditions
- 2018
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Ingår i: Catalysis Science and Technology. - : Royal Society of Chemistry (RSC). - 2044-4753 .- 2044-4761. ; 8:10, s. 2686-2696
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Tidskriftsartikel (refereegranskat)abstract
- The effect of support material and chemical state of Rh for Rh/Al2O3 and Rh/SiO2 model catalysts during CO2 hydrogenation were studied by a combined array of in situ characterisation techniques including diffuse reflectance infrared Fourier transform spectroscopy, energy-dispersive X-ray absorption spectroscopy and high-energy X-ray diffraction at 250-350 °C and atmospheric pressure. The CO2 methanation proceeds via intermediate formation of adsorbed CO species on metallic Rh likely followed by their hydrogenation to methane. Linearly-bonded CO species is suggested to be a more active precursor in the hydrogenation compared to the bridge-bonded species, which seems to relate to particle size effects: for larger particles mainly the formation of inactive bridge-bonded CO species takes place. Further, analysis of the chemical state of Rh during reaction conditions reveal a minor formation of RhOx from dissociation of CO2 , which is a consequence of the increased activity observed over Rh/Al2O3 catalyst.
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| 7. |
- Wang, Xueting, 1991, et al.
(författare)
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Copper-modified zeolites and silica for conversion of methane to methanol
- 2018
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Ingår i: Catalysts. - : MDPI AG. - 2073-4344. ; 8:11
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Tidskriftsartikel (refereegranskat)abstract
- Powder materials containing copper ions supported on ZSM-5 (Cu-Zeolite Socony Mobil-5) and SSZ-13 (Cu-Standard Oil synthesised zeolite-13), and predominantly CuO nanoparticles on amorphous SiO2 were synthesised, characterised, wash-coated onto ceramic monoliths and, for the first time, compared as catalysts for direct conversion of methane to methanol (DCMM) at ambient pressure (1 atm) using O2, N2 O and NO as oxidants. Methanol production was monitored and quantified using Fourier transform infrared spectroscopy. Methanol is formed over all monolith samples, though the formation is considerably higher for the copper-exchanged zeolites. Hence, copper ions are the main active sites for DCMM. The minor amount of methanol produced over the Cu/SiO2 sample, however, suggests that zeolites are not the sole substrate that can host those active copper sites but also silica. Further, we present the first ambient pressure in situ infrared spectroscopic measurements revealing the formation and consumption of surface methoxy species, which are considered to be key intermediates in the DCMM reaction.
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| 8. |
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| 9. |
- Dahlin, Sandra, et al.
(författare)
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Effect of biofuel- and lube oil-originated sulfur and phosphorus on the performance of Cu-SSZ-13 and V2O5-WO3/TiO2 SCR catalysts
- 2021
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Ingår i: Catalysis Today. - : Elsevier B.V.. - 0920-5861 .- 1873-4308. ; 360, s. 326-339
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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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| 10. |
- Englund, Johanna, 1988, et al.
(författare)
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Deactivation of a Pd/Pt Bimetallic Oxidation Catalyst Used in a Biogas-Powered Euro VI Heavy-Duty Engine Installation
- 2019
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Ingår i: Catalysts. - : MDPI. - 2073-4344. ; 9:12
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Tidskriftsartikel (refereegranskat)abstract
- The reduction of anthropogenic greenhouse gas emissions is crucial to avoid further warming of the planet. We investigated how effluent gases from a biogas powered Euro VI heavy-duty engine impact the performance of a bimetallic (palladium and platinum) oxidation catalyst. Using synthetic gas mixtures, the oxidation of NO, CO, and CH4 before and after exposure to biogas exhaust for 900 h was studied. The catalyst lost most of its activity for methane oxidation, and the activity loss was most severe for the inlet part of the aged catalyst. Here, a clear sintering of Pt and Pd was observed, and higher concentrations of catalyst poisons such as sulfur and phosphorus were detected. The sintering and poisoning resulted in less available active sites and hence lower activity for methane oxidation.
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