N2O decomposition over iron-containing zeolites prepared by different methods: a comparison of the reaction mechanism

Pirngruber, Gerhard D.; Luechinger, Marco; Roy, Pijus K.; Cecchetto, Andrea; Smirniotis, Panagiotis G.

doi:10.1016/j.jcat.2004.03.031

Cited by 107 publications

(77 citation statements)

References 52 publications

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“…As a result we concluded that the pre-treatment of the zeolite affects the surface oxygen formation. Moreover, we found further evidence that different surface oxygen species exist which differ in thermal stability and reactivity, in agreement to results of other groups [8,13,16,[20][21][22][23]32].…”

Section: Introductionsupporting

confidence: 92%

“…As shown by other research groups, these species differ in stability and reactivity, particularly, in zeolites with high iron contents [13,[20][21][22][23]32], but also with low iron contents [8,[16][17][18]32]. For example, recent pulse studies in the TAP reactor published in Ref.…”

Section: Step Techniquementioning

confidence: 91%

“…(3)) should not be excluded in these considerations, as shown by results in Refs. [2,29,31,32]. Pulse experiments may suppress this reaction due to much lower N 2 O concentrations in the gas phase than under steady state conditions.…”

Section: Kinetics Of the Total N 2 O Decompositionmentioning

confidence: 99%

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Experimental techniques for investigating the surface oxygen formation in the N2O decomposition on Fe-MFI zeolites

Ateş¹,

Reitzmann²

2007

Chemical Engineering Journal

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Several experimental techniques were used to investigate the formation of surface oxygen in the N 2 O decomposition on an Fe-MFI zeolite. These techniques consisted of multipulse and step experiments as transient methods at ambient pressure and experiments in a closed set-up of Panov and co-workers at strongly reduced pressure. The total amount of surface oxygen determined through multipulse experiments was in the range of the amount obtained in the vacuum set-up at 523 K (40-50 mol O g −1 catalyst ). In contrast, the step technique revealed considerably higher values, up to 110 mol O g −1 catalyst , indicating an accumulation of oxygen in the zeolite. This phenomenon might also be responsible for the observation that higher reaction temperatures increase the total amount of surface oxygen, which can be deposited in the zeolite. In contrast to experiments in the vacuum set-up, the temperature-programmed desorption after multipulse and step experiments shows the presence of various oxygen species differing in thermal stability. The influence of temperature on the rate of surface oxygen formation was determined from step and vacuum experiments. The results of the step experiments lead to a lower activation energy, 14 kJ mol −1 , than the experiments in the vacuum set-up (49 kJ mol −1 ), probably due to sorption and mass transfer effects. Comparing the rate of surface oxygen formation and of total N 2 O decomposition reveals that the former is very fast and not rate determining for the latter. Furthermore, the rate of total N 2 O decomposition seems to be inhibited by adsorbed N 2 O, detected in the transient experiments. This observation is considered in an adequate kinetic model.

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Section: Introductionsupporting

confidence: 92%

Section: Step Techniquementioning

confidence: 91%

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Experimental techniques for investigating the surface oxygen formation in the N2O decomposition on Fe-MFI zeolites

Ateş¹,

Reitzmann²

2007

Chemical Engineering Journal

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“…Other minerals, such as feldspar, may only contain traces of Fe, while quartz anhydrite, gypsum and halite do not contribute any Fe to the reservoir rock. Although analcime itself does not contain Fe, zeolites are known for their ability to bind Fe (Pirngruber et al 2004). Origin of the iron and past Fe-cycling…”

Section: Discussionmentioning

confidence: 99%

Mineralogical and geochemical analysis of Fe-phases in drill-cores from the Triassic Stuttgart Formation at Ketzin CO2 storage site before CO2 arrival

et al. 2017

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Reactive iron (Fe) oxides and sheet silicatebound Fe in reservoir rocks may affect the subsurface storage of CO 2 through several processes by changing the capacity to buffer the acidification by CO 2 and the permeability of the reservoir rock: (1) the reduction of threevalent Fe in anoxic environments can lead to an increase in pH, (2) under sulphidic conditions, Fe may drive sulphur cycling and lead to the formation of pyrite, and (3) the leaching of Fe from sheet silicates may affect silicate diagenesis. In order to evaluate the importance of Fe-reduction on the CO 2 reservoir, we analysed the Fe geochemistry in drill-cores from the Triassic Stuttgart Formation (Schilfsandstein) recovered from the monitoring well at the CO 2 test injection site near Ketzin, Germany.The reservoir rock is a porous, poorly to moderately cohesive fluvial sandstone containing up to 2-4 wt% reactive Fe. Based on a sequential extraction, most Fe falls into the dithionite-extractable Fe-fraction and Fe bound to sheet silicates, whereby some Fe in the dithionite-extractable Fe-fraction may have been leached from illite and smectite. Illite and smectite were detected in core samples by X-ray diffraction and confirmed as the main Fe-containing mineral phases by X-ray absorption spectroscopy. Chlorite is also present, but likely does not contribute much to the high amount of Fe in the silicate-bound fraction. The organic carbon content of the reservoir rock is extremely low (\0.3 wt%), thus likely limiting microbial Fe-reduction or sulphate reduction despite relatively high concentrations of reactive Fe-mineral phases in the reservoir rock and sulphate in the reservoir fluid. Both processes could, however, be fuelled by organic matter that is mobilized by This article is part of a Topical Collection in Environmental Earth Sciences on ''Subsurface Energy storage'', guest-edited by

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“…Many efforts have been made to develop end-of-pipe technologies to mitigate N 2 O emissionfromanthropogenic sources,such asadipic acid production and nitric acid manufacture. An effective way to minimize the impact of N 2 O on the environment is to catalytically decompose N 2 O to environment-friendly N 2 and O 2 [3][4][5][6][7].…”

Section: Introductionmentioning

confidence: 99%

Fe-mordenite/cordierite monolith for the catalytic decomposition of nitrous oxide

Zhou¹,

Li²,

Cheng³

et al. 2009

Ceramics International

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Mordenite zeolites were coated on cordierite support by in situ hydrothermal method or dip-coating method. The mordenite/cordierite was characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM) techniques and their stability was studied. The mordenite/ cordierite monolith prepared by in situ synthesis showed much better stability than that prepared by dip-coating. Iron was introduced into mordenite/cordierite by ion exchange and Fe-mordenite/cordierite catalyst was prepared. Fe-mordenite/cordierite prepared from in situ synthesis exhibited good activity and stability for N 2 O catalytic decomposition, with great potential for future application. #

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N2O decomposition over iron-containing zeolites prepared by different methods: a comparison of the reaction mechanism

Cited by 107 publications

References 52 publications

Experimental techniques for investigating the surface oxygen formation in the N2O decomposition on Fe-MFI zeolites

Experimental techniques for investigating the surface oxygen formation in the N2O decomposition on Fe-MFI zeolites

Mineralogical and geochemical analysis of Fe-phases in drill-cores from the Triassic Stuttgart Formation at Ketzin CO2 storage site before CO2 arrival

Fe-mordenite/cordierite monolith for the catalytic decomposition of nitrous oxide

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