The effect of SO2 on the oxidation of NO over Fe-MFI and Fe-ferrierite catalysts made by solid-state ion exchange

Giles, R.G.F.; Cant, Noel W.; Kögel, M.; Turek, Thomas; Trimm, D.L.

doi:10.1016/s0926-3373(99)00136-8

Cited by 25 publications

(19 citation statements)

References 21 publications

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“…In fact, the energies corresponding to the cycle on FeOH resemble strongly those of FeONO as the active site for which the conclusion was already drawn that it is less active than FeO. This finding is in agreement with the experimental results of Giles et al and Kröcher et al, who stated an inhibiting influence of water on the NO oxidation.…”

Section: Resultssupporting

confidence: 91%

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Theoretical Investigation of the Mechanism of the Oxidation of Nitrogen Oxide on Iron-Form Zeolites in the Presence of Water

Brüggemann

Keil

2011

J. Phys. Chem. C

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The oxidation of NO to NO2 by oxygen and the influence of water have been investigated on a portion of the Fe−ZSM5 which contains 5 T atoms by using the density functional theory. The iron was considered to be a mononuclear species. For the main reaction pathway it is most likely that NO initially adsorbs on Z−[FeO]+, forming the nitrite Z−[FeONO]+ which includes a spin change from the septet to the quintet potential energy surfaces (PES). The adsorption of oxygen and the desorption of NO2 leads to Z−[FeO2]+ which is attacked by NO from the gas phase. Within another spin change from the septet to the quintet PES, the ligand with the sequence -OONO is formed of which NO2 desorbs. The latter step is rate-limiting for the overall mechanism. A final spin change restores the initial active site on the sextet PES. At the same time, the nitrite Z−[FeO2N]+ and the nitrate Z−[FeO2NO]+ are rapidly formed and block the active site. Water leads to the formation of, first, a dihydroxylated iron Z−[HOFeOH]+ and after the reaction with NO or NO2 to nitrous and nitric acid, respectively, together with monohydroxylated iron Z−[FeOH]+. The dihydroxylated iron is inactive for the oxidation of NO, and the monohydroxylated exhibits a reduced activity as compared to Z−[FeO]+. Further removal of hydroxyl groups by reaction with NO x is also accessible, restoring nonhydroxylated iron sites. Furthermore, water also potentially reacts directly with the surface nitrite and nitrate, leading to nitrous and nitric acid. This explains the phenomena of a short-term release of significant amounts of NO2 upon water addition in transient experiments. The results of this work are in agreement with the experimental literature and account for many observed phenomena.

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Section: Resultssupporting

confidence: 91%

“…Kröcher et al and Giles et al found water to significantly inhibit the oxidation of nitrogen oxide. Furthermore, there is agreement in the literature − that the NO oxidation is the rate-limiting step of the SCR, which itself produces water.…”

Section: Resultsmentioning

confidence: 98%

Theoretical Investigation of the Mechanism of the Oxidation of Nitrogen Oxide on Iron-Form Zeolites in the Presence of Water

Brüggemann

Keil

2011

J. Phys. Chem. C

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“…The reduction peak at higher temperature of 150 8C is attributed to the reduction of amorphous RuO x with Ru-support interaction while reduction peak at the lower temperature of 105 8C is attributed to the reduction of highly dispersed amorphous RuO x . The reduction peak at 75 8C in the TPR profile of reference amorphous RuO 2 sample should be attributed to the reduction of atomically dispersed Ru n+ [28]. As seen in Fig.…”

Section: Effects Of Supports and Ru Loadings On No Oxidation Over Ru mentioning

confidence: 76%

Oxidation of nitric oxide to nitrogen dioxide over Ru catalysts

Cheng

et al. 2009

Applied Catalysis B: Environmental

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“…The formed SO 3 may not only occupy the active sites for NO oxidation but also cover the support materials by forming sulfates. As a result, serious deactivation by SO 2 is generally observed on catalysts for NO oxidation [36][37][38]. In this work, SO 2 -resistant TiO 2 is selected as the support for platinum and the formation sulfates on support is greatly prohibited.…”

Section: Catalytic Performance For No Oxidationmentioning

confidence: 99%

Catalytic oxidation of NO over TiO2 supported platinum clusters I. Preparation, characterization and catalytic properties

Shen

Cheng

et al. 2010

Applied Catalysis B: Environmental

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The effect of SO2 on the oxidation of NO over Fe-MFI and Fe-ferrierite catalysts made by solid-state ion exchange

Cited by 25 publications

References 21 publications

Theoretical Investigation of the Mechanism of the Oxidation of Nitrogen Oxide on Iron-Form Zeolites in the Presence of Water

Theoretical Investigation of the Mechanism of the Oxidation of Nitrogen Oxide on Iron-Form Zeolites in the Presence of Water

Oxidation of nitric oxide to nitrogen dioxide over Ru catalysts

Catalytic oxidation of NO over TiO2 supported platinum clusters I. Preparation, characterization and catalytic properties

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