| 1. |
- Di, Mengqiao, 1994, et al.
(författare)
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Chasing PtO x species in ceria supported platinum during CO oxidation extinction with correlative operando spectroscopic techniques
- 2022
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Ingår i: Journal of Catalysis. - : Elsevier BV. - 0021-9517 .- 1090-2694. ; 409, s. 1-11
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Tidskriftsartikel (refereegranskat)abstract
- Industrially relevant, highly dispersed, Pt/ceria and reference Pt/alumina catalysts with narrow Pt particle size distributions have been prepared, characterised ex situ and studied for CO oxidation by operando infrared and X-ray absorption spectroscopy. At high CO conversions, spectator CO ad-species on ionic platinum are observed while the CO oxidation proceeds on Pt particles in a high oxidation state exhibiting significant Pt[sbnd]O coordination. During the protracted catalytic extinction, the CO coverage builds up gradually while the Pt oxidation state and Pt[sbnd]O coordination remain high because of interactions with ceria. The observed CO oxidation at high CO coverage is suggested to involve sites at the platinum-ceria boundary that cannot be CO self-poisoned. This behaviour is in stark contrast to that of Pt/alumina, which shows removal of platinum oxides formed during CO oxidation and the classical drop in catalytic activity caused by rapid CO self-poisoning when reaching a critical temperature.
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| 2. |
- Di, Mengqiao, 1994, et al.
(författare)
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Why nitrogen oxide inhibits CO oxidation over highly dispersed platinum ceria catalysts
- 2024
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Ingår i: Catalysis Today. - 0920-5861. ; 426
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Tidskriftsartikel (refereegranskat)abstract
- The influence of nitrogen oxide on the lean CO oxidation activity of highly dispersed Pt/ceria and reference Pt/alumina catalysts has been studied by kinetic measurements and infrared spectroscopic characterization. Co-feeding of nitrogen oxide leads to the formation of nitrates on the supports that induce a highly oxidized character of the Pt sites and in the case of Pt/ceria, inhibit ceria lattice oxygens to react with CO adsorbed on Pt rim sites via a Mars-van Krevelen mechanism below the ignition temperature. The build-up of nitrates below the light-off temperatures is faster when CO is present in the feed. Above the light-off temperatures, carbonates replace the nitrates while the catalytic activity remains high.
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| 3. |
- Martin, Natalia Mihaela, 1984, et al.
(författare)
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A LEIS and in situ XAS study of supported Pd-Pt catalysts for CH4 oxidation
- 2016
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Konferensbidrag (övrigt vetenskapligt/konstnärligt)abstract
- It is of vital importance to remove methane (CH4) from the exhausts of natural gas and biogas fueled engines as CH4 is a strong greenhouse gas. So far Pd-based catalysts have been used almost exclusively but their high sensitivity to sulfur and water pushes research to explore other materials. Among these are Pd-Pt catalysts [1-4], which exhibit a slight increase in CH4 oxidation activity with time and higher long-term stability than the Pd-only counterpart [5-7]. Still, however, little is known about the oxidation-reduction behaviour of the Pd-Pt nanoclusters and how this impacts the catalytic activity. This study aims at increase the understanding of the catalytic activity of Al2O3-supported Pd-Pt nanoclusters for low-temperature CH4 oxidation under transient, although generally lean, conditions.
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| 4. |
- 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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| 5. |
- Martin, Natalia M., et al.
(författare)
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CO Oxidation and Site Speciation for Alloyed Palladium-Platinum Model Catalysts Studied by in Situ FTIR Spectroscopy
- 2017
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 121:47, s. 26321-26329
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Tidskriftsartikel (refereegranskat)abstract
- In situ Fourier transform infrared spectroscopy was used to study transient CO oxidation over a series of bimetallic Pd-Pt catalysts with different Pd:Pt molar ratios. The catalysts were found to contain both alloyed PdPt nanoparticles (particle sizes 25-35 nm) and monometallic Pd nanoparticles (sizes below 10 nm). For oxygen-free conditions, CO reduces the surface while simultaneously function as a chemical probe molecule whereby the CO adsorption sites can be characterized. Under these conditions, it is shown that adsorbed carbonyl species form both on the Pd and Pt. On platinum, CO adsorbs predominantly linearly on top, whereas on palladium it adsorbes in bridged configurations. This behavior is used for site speciation of the catalysts. The spectra from the bimetallic Pd-Pt catalysts are more complicated than a direct superposition of the spectra for the monometallic catalysts as a consequence of alloy formation and enrichment of Pd at the surface of the reduced catalysts. The temperature-programmed CO oxidation results show that the addition of Pd to the Pt catalyst supported on alumina shifts the CO-poisoned state to lower temperatures, therefore increasing the temperature range for the CO oxidation at low temperatures.
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| 6. |
- Martin, Natalia Mihaela, 1984, et al.
(författare)
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CO Oxidation and Site Speciation for Alloyed Pd-Pt Model Catalysts Studied by In Situ FTIR Spectroscopy
- 2017
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Ingår i: Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 121:47, s. 26321-26329
-
Tidskriftsartikel (refereegranskat)abstract
- In situ Fourier transform infrared spectroscopy was used to study transient CO oxidation over a series of bimetallic Pd-Pt catalysts with different Pd:Pt molar ratios. The catalysts were found to contain both alloyed PdPt nanoparticles (particle sizes 25-35 nm) and monometallic Pd nanoparticles (sizes below 10 nm). For oxygen-free conditions, CO reduces the surface while simultaneously function as a chemical probe molecule whereby the CO adsorption sites can be characterised. Under these conditions it is shown that adsorbed carbonyl species form both on the Pd and Pt. On platinum, CO adsorbs predominantly linearly on top, whereas on palladium it adsorbes in bridged configurations. This behaviour is used for site speciation of the catalysts. The spectra from the bimetallic Pd-Pt catalysts are more complicated than a direct superposition of the spectra for the monometallic catalysts as a consequence of alloy formation and enrichment of Pd at the surface of the reduced catalysts. The temperature programmed CO oxidation results show that the addition of Pd to the Pt catalyst supported on alumina shifts the CO-poisoned state to lower temperatures therefore increasing the temperature range for the CO oxidation at low temperatures.
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| 7. |
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| 8. |
- Martin, Natalia Mihaela, 1984, et al.
(författare)
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Study of methane oxidation over alumina supported Pd-Pt catalysts using operando DRIFTS/MS and in situ XAS techniques
- 2017
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Ingår i: Catalysis, Structure and Reactivity. - 2055-0758. ; 3:1-2, s. 24-32
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Tidskriftsartikel (refereegranskat)abstract
- Methane oxidation over Pd–Pt/Al2O3 model catalysts calcined at three different conditions is investigated using operando diffuse reflectance infrared Fourier transform spectroscopy and mass spectrometry, and in situ X-ray absorption spectroscopy while cycling the feed gas stoichiometry between lean (net-oxidising) and rich (net-reducing) conditions. When calcined in air, alloy Pd–Pt nanoparticles are present only on catalysts subjected to elevated temperature (800 ◦C) whereas calcination at lower temperature (500◦C) leads to segregated Pt and Pd nanoparticles on the support. Here, we show that the alloy Pd–Pt nanoparticles undergo reversible changes in surface structure and composition during transient methane oxidation exposing a PdO surface during lean conditions and a metallic Pd–Pt surface (Pd enriched) under rich conditions. Alloyed particles seem more active for methane oxidation than their monometallic counterparts and, furthermore, an increased activity for methane oxidation is clearly observed under lean conditions when PdO has developed on the surface, analogous to monometallic Pd catalysts. Upon introducing rich conditions, partial oxidation of methane dominates over total oxidation forming adsorbed carbonyls on the noble metal particles. The carbonyl spectra for the three samples show clear differences originating from different surfaces exposed by alloyed vs. non-alloyed particles. The kinetics of the noble metal oxidation and reduction processes as well as carbonyl formation during transient methane oxidation are discussed.
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| 10. |
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