| 1. |
- Feizie Ilmasani, Rojin, 1989, et al.
(författare)
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Deactivation of phosphorus-poisoned Pd/SSZ-13 for the passive adsorption of NOx
- 2022
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Ingår i: Journal of Environmental Chemical Engineering. - : Elsevier BV. - 2213-3437 .- 2213-2929. ; 10:3
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Tidskriftsartikel (refereegranskat)abstract
- Automotive catalysts can be exposed to various poisonous substances that can cause physical or chemical deactivation. One of such poisons is phosphorous, which originates from lubricant oils. This study focuses on the phosphorus deactivation of Pd/SSZ-13 used as a passive NOx adsorber (PNA). A clear deactivation caused by phosphorus was observed, and it was increased by increasing the content of phosphorous. It was concluded that phosphorous can cause both physical and chemical deactivation. This was evident from XPS analysis, where the presence of phosphorus pentoxide (P2O5) causes physical deactivation whereas metaphosphate (PO3-) and phosphate (PO43-) cause chemical deactivation. Also, it was shown that metaphosphates (PO3-) become the dominant phosphorous species at higher P concentrations. Lesser amounts of O2 were released in P-poisoned Pd/SSZ-13, as was found in oxygen TPD when increasing the P concentration, due to the presence of more PO3- species. Furthermore, XRD and 27Al NMR analyses revealed that phosphorus also interacted with alumina in the zeolite framework by forming Al-O-P species; this was also supported by SEM-EDX, where there was a clear overlap of P with Al and Pd spectra. DRIFTS analysis showed that OH groups in contact with the zeolite structure became contaminated by phosphorus and caused a chemical deactivation of Pd/SSZ-13. It was also found that, during multiple cycles, the PNA capacity decreased for phosphorus-poisoned samples. This was caused by the transformation of P2O5, which causes physical blocking, to PO3-, which interacts chemically with the palladium species.
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| 2. |
- Feizie Ilmasani, Rojin, 1989, et al.
(författare)
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Investigation of CO Deactivation of Passive NOx Adsorption on La Promoted Pd/BEA
- 2022
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Ingår i: Emission Control Science and Technology. - : Springer Science and Business Media LLC. - 2199-3629 .- 2199-3637. ; 8:1-2, s. 63-77
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Tidskriftsartikel (refereegranskat)abstract
- Passive NOx adsorption (PNA) is a method, in which NOx can be stored at low temperatures and released at higher temperatures where the urea decomposition is functional during selective catalytic reduction (i.e., above 180–200 °C). We have studied the promotion of Pd/BEA with La as a PNA in the presence of high CO concentration. Both the reference and promoted samples exhibited a significant loss of NOx adsorption/desorption capacity after multiple cycles using 4000 ppm CO. However, already after 5 cycles, 99% of the NOx released between 200 and 400 °C was lost for Pd/BEA, compared to only 64% for Pd-La/BEA, which thereafter was stable. XPS and O2-TPD clearly showed that the Pd species were influenced by La. The PNA deactivation in the presence of CO could be related to Pd reduction followed by migration and the formation of more PdOx clusters, as observed by O2-TPD analysis. Interestingly, significantly more PdOx clusters formed on Pd/BEA after 10 cycles compared to Pd-La/BEA.
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| 3. |
- Ho, Hoang Phuoc, 1983, et al.
(författare)
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Role of the supports during phosphorus poisoning of diesel oxidation catalysts
- 2023
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Ingår i: Chemical Engineering Journal. - 1385-8947. ; 468
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Tidskriftsartikel (refereegranskat)abstract
- Phosphorus (P) poisoning is one of the main factors accounting for the deactivation of diesel oxidation catalysts (DOC) apart from sulfur poisoning and sintering of the Pt active sites. This study compares the impact of P with loading up to 2.4 wt% on the catalytic performance of monometallic and bimetallic Pt-Pd catalysts using alumina and high silica BEA zeolites as the supports. P poisoning caused deactivation for CO, C3H6, C3H8 and NO oxidation; however, the degree of the impact of P in terms of temperatures at which 50% of the component is converted (T50) depends not only on the types of the active phase (Pt and Pt-Pd) but also on the types of supports (alumina and BEA zeolite). The influence of P impregnation on the textural properties of the materials is more significant for zeolite than alumina-based catalysts, which is in line with the activity measurements. A weak interaction between P and high silica zeolite resulted in the formation of a prominent fraction of P2O5 in the P-Pt/BEA, whereas a strong binding between P and alumina accounted for a dominant fraction of phosphate in the P-Pt/Al2O3 as revealed by XPS and NMR measurements. Phosphorus compounds partially covered the available surface of the active sites and this lowered the catalytic activity. For alumina-based catalysts, P mainly reacted with the support and only deactivated a part of the active noble metals. Whereas, for zeolite-based catalysts, P existed mainly in the form of phosphorus oxides that significantly blocked the catalyst surface and thereby deactivated more of the available active sites than that on alumina-based materials, which is consistent with the CO chemisorption data.
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| 4. |
- Ho, Hoang Phuoc, 1983, et al.
(författare)
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The effect of Pt/Pd ratio on the oxidation activity and resistance to sulfur poisoning for Pt-Pd/BEA diesel oxidation catalysts with high siliceous content
- 2022
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Ingår i: Journal of Environmental Chemical Engineering. - : Elsevier BV. - 2213-3437 .- 2213-2929. ; 10:4
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Tidskriftsartikel (refereegranskat)abstract
- This study investigates the effect of the Pt/Pd ratio on the oxidation activity and sulfur poisoning/regeneration of diesel oxidation catalysts (DOC) using beta zeolites with high siliceous content as support. Formation of Pt-Pd alloy leads to contraction of the cell lattice of Pt in the bimetallic catalysts, improving not only the sintering resistance of Pt but also retaining a high fraction of Pd in Pd2+ form. Moreover, the Pt-Pd alloy also improves the oxidation resistance of the particles, which enhances the activity of the catalysts for CO and C3H6 oxidation. Bimetallic catalysts also favor NO reduction at a lower temperature than the monometallic Pt although they showed lower values for the absolute conversion of NO due to a decrease in the total number of the Pt active sites. In addition, the bimetallic catalysts significantly improved the sulfur resistance as compared to the monometallic Pd catalyst. Moreover, the bimetallic catalysts could easily recover their activity for NO and C3H6 oxidation by thermal treatment either in lean conditions or in H2. The reduction with H2 was necessary to recover completely the activity of the CO and C3H8 oxidation.
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| 5. |
- Yao, Dawei, 1991, et al.
(författare)
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Deciphering SO2 poisoning mechanisms for passive NOx adsorption: A kinetic modeling approach and development of a high-resistance catalyst
- 2024
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Ingår i: Chemical Engineering Journal. - 1385-8947. ; 487
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Tidskriftsartikel (refereegranskat)abstract
- Passive NOx adsorption (PNA) is a promising technology aimed at reducing NOx emissions from vehicles during the cold start phase of the engine. This work investigated the SO2 poisoning mechanism of PNA through a combination of experimental research and kinetic modeling, leading to the development of a novel PNA sample with high resistance to SO2 poisoning. Pd/SSZ-13 samples were synthesized using different drying conditions, revealing that samples dried at room temperature showed lower degradation (10 %) compared to those dried at 80 °C (26 %). Investigation into the degradation revealed that ion-exchanged Pd sites with a hydroxyl group were more resistant to SO2 poisoning than other Pd sites. It is also found that SO2 aids in NOx storage on Pd sites, enhancing the PNA performance. A kinetic model was developed to describe the SO2 poisoning behavior and its influence on NOx storage. The model, which was verified under various conditions, effectively simulated the PNA behavior and SO2 poisoning of Pd/SSZ-13.
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| 6. |
- Yao, Dawei, 1991, et al.
(författare)
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Enhanced CO resistance of Pd/SSZ-13 for passive NOx adsorption
- 2023
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Ingår i: Chemical Engineering Journal. - : Elsevier BV. - 1385-8947. ; 460
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Tidskriftsartikel (refereegranskat)abstract
- Passive NOx adsorption (PNA) is a novel technology to control NOx emissions during cold start. However, the recent generation of PNA material, Pd/zeolite, suffers from major degradation under high CO concentrations. In this work, we developed a novel form of Pd/SSZ-13 by using a freeze-drying process after incipient wetness impregnation. This Pd/SSZ-13 showed a better stability than the sample synthesized by the common process. Several characterization measurements were conducted and it was found that the Pd sites on the freeze-dried sample were more resistant towards CO-induced agglomeration. By combing in-situ characterization and kinetic modeling, we found that the freeze-dried Pd/SSZ-13 had more ion-exchanged Pd sites, which provided greater resistance towards the CO-induced Ostwald ripening process, and consequently suppressed the sintering behavior under a high CO concentration. This material offers a potentially improved stability of PNAs under extremely high CO concentration pulses from incomplete diesel combustion during engine cold start.
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| 7. |
- Yao, Dawei, 1991, et al.
(författare)
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Insight into CO induced degradation mode of Pd/SSZ-13 in NOx adsorption and release: Experiment and modeling
- 2022
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Ingår i: Chemical Engineering Journal. - : Elsevier BV. - 1385-8947. ; 439
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Tidskriftsartikel (refereegranskat)abstract
- Passive NOx adsorption (PNA) on Pd zeolites is an important technique to remove NOx during the cold start of the engine. However, the stability of Pd zeolites under high concentrations of CO is still challenging in multiple cold starts of an engine. Herein, we illustrate the CO-induced degradation mechanism of Pd zeolite by combining experiments and kinetic models. Pd/SSZ-13 has been used in multicycle processes containing NOx adsorption at low temperature and temperature programmed desorption, which represents the PNA degradation in multiple cold start periods. A kinetic model was developed to describe the NOx storage and degradation behavior of Pd/SSZ-13. Both experimental and modelling observations suggested that two Pd sintering modes are occurring under high CO concentration (4000 ppm), namely Ostwald ripening and particle migration. Apart from the degradation behavior, this model is also adequate for describing multi-cycle NOx storage and release behavior under low CO concentration.
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| 8. |
- Yao, Dawei, 1991, et al.
(författare)
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Kinetic modeling of CO assisted passive NOx adsorption on Pd/SSZ-13
- 2022
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Ingår i: Chemical Engineering Journal. - : Elsevier BV. - 1385-8947. ; 428
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Tidskriftsartikel (refereegranskat)abstract
- Passive NOx adsorption (PNA) has been recently developed as a promising technology for controlling the NOx emissions during the cold start period. In this work, we illustrate a CO-assisted mechanism by combining experimental and kinetic modeling studies. Pd/SSZ-13 has been synthesized, characterized and evaluated as a PNA in low-temperature NOx adsorption and temperature program desorption cycles, to represent multiple cold start periods. The gas compositions were also systemically changed, where both the effect of varying NOx and CO feed was evaluated in the presence of high water and oxygen contents. A kinetic model was developed to simulate the profiles of NO and NO2, including three initial Pd sites (Z-Pd(II)Z-, Z-[Pd(II)OH]+ and PdO). It is concluded from XPS and in situ DRIFTS experiments, flow reactor measurements and modelling observations that CO reduces Pd(II) species to Pd(I)/Pd(0) species, which increases the stability of the stored NOx species, resulting in a release above the urea dosing temperature. The model could well describe the experimental features, including the effect of CO. In addition, the model was used for full-scale catalytic converter simulations.
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