Browsing by Subject "Adsorption experiment"
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Item Open Access Fe promoted NOx storage materials: structural properties and NOx uptake(American Chemical Society, 2010) Kayhan, E.; Andonova, S. M.; Şentürk, G. S.; Chusuei, C. C.; Ozensoy, E.Fe promoted NOx storage materials were synthesized in the form of FeOx/BaO/Al2O3 ternary oxides with varying BaO (8 and 20 wt %) and Fe (5 and 10 wt %) contents. Synthesized NOx storage materials were investigated via TEM, EELS, BET, FTIR, TPD, XRD, XPS, and Raman spectroscopy, and the results were compared with the conventional BaO/Al2O3 NOx storage system. Our results suggest that the introduction of Fe in the BaO/Al2O3 system leads to the formation of additional NOx storage sites which store NOx mostly in the form of bidentate nitrates. NO2 adsorption experiments at 323 K via FTIR indicate that, particularly in the early stages of the NOx uptake, the NOx storage mechanism is significantly altered in the presence of Fe sites where a set of new surface nitrosyl and nitrite groups were detected on the Fe sites and the surface oxidation of nitrites to nitrates is significantly hindered with respect to the BaO/Al2O3 system. Evidence for the existence of both Fe3+ as well as reduced Fe2+/(3-x)+ sites on the freshly pretreated materials was detected via EELS, FTIR, Raman, and XRD experiments. The influence of the Fe sites on the structural properties of the synthesized materials was also studied by performing ex situ annealing protocols within 323-1273 K followed by XRD and Raman experiments where the temperature dependent changes in the morphology and the composition of the surface domains were analyzed in detail. On the basis of the TPD data, it was found that the relative stability of the stored NOx species is influenced by the morphology of the Ba and Fe containing NOx-storage domains. The relative stabilities of the investigated NOx species were found to increase in the following order: N2O3/NO+ < nitrates on γ-Al2O3 < surface nitrates on BaO < bidentate nitrates on FeOx sites < bulk nitrates on BaO.Item Open Access Sulfur poisoning and regeneration behavior of perovskite-based NO oxidation catalysts(Springer New York LLC, 2017) Kurt M.; Say, Z.; Ercan, K. E.; Vovk, E. I.; Kim, C. H.; Ozensoy, E.SOxuptake and release properties of LaMnO3, Pd/LaMnO3, LaCoO3and Pd/LaCoO3perovskites were investigated via in situ Fourier transform infrared (FTIR) spectroscopy, temperature programmed desorption and X-ray photoelectron spectroscopy. Sulfation of the perovskite leads to the formation of surface sulfite/sulfate and bulk-like sulfate species. Pd addition to LaMnO3and LaCoO3significantly increases the sulfur adsorption capacity. Pd/LaMnO3sample accumulates significantly more sulfur than LaMnO3; however it can also release a larger fraction of the accumulated SOxspecies in a reversible fashion at elevated temperatures in vacuum. This is not the case for Co-based materials, where thermal regeneration of bulk sulfates on poisoned LaCoO3and Pd/LaCoO3is extremely ineffective under similar conditions. However, in the presence of an external reducing agent such as H2(g), Pd/LaMnO3requires much lower temperature (873�K) for complete sulfur regeneration as compared to that of Pd/LaCoO3(973�K). Sequential CO and SOxadsorption experiments performed via in situ FTIR indicate that in the presence of carbonyls and/or carbonates, Pd adsorption sites may have a stronger affinity for SOxas compared to that of the perovskite surface, particularly in the early stages of sulfur poisoning.