Mechanism and Kinetics of the Selective NO Reduction over Co-ZSM-5 Studied by the SSITKA Technique

Sadovskaya, E. M.; Suknev, A.P.; Пинаева, Л. Г.; Goncharov, V. B.; Бальжинимаев, Б. С.; Chupin, C; Mirodatos, C.

doi:10.1006/jcat.2001.3256

Cited by 23 publications

(31 citation statements)

References 21 publications

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“…The conversion of methane was 30% for the feed concentration considered (0.6%). More data is given in [13].…”

Section: Main Results Of the Ssitka Studymentioning

confidence: 99%

“…The initial values of the equilibrium constants of NO adsorption on Co 2+ and NO 2 d+ formation have been calculated according to data obtained by SSITKA [12,13]. Since NO 2 adsorbed species have the same molecular structure and the same scheme of adsorption as NO 2 d+ species -except a second anchoring point -we attributed a similar initial value to the equilibrium constant as NO 2 d+ .…”

Section: Comparison Between Two Models a And Bmentioning

confidence: 99%

“…The various parameters were determined by minimizing root-mean-square deviation of experimental data from calculated ones [12,13].…”

Section: Numerical Analysis Of Ssitka Responsesmentioning

confidence: 99%

“…In this paper, we will resume the data obtained from DRIFT and SSITKA investigation, already published in [10][11][12][13] and present new data from a formal steady-state kinetic analysis (SSKA), in view to compare and discuss the surface coverages obtained from these various methodologies.…”

Section: Introductionmentioning

confidence: 96%

“…Changes in isotopic concentration after the 14 N 16 O/ 15 N 18 O switch under SCR conditions. Experimental data and modelled curves[13].…”

mentioning

confidence: 99%

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Can isotopic transient and formal steady-state kinetics lead to a converging surface chemistry analysis? Case study on the selective reduction of NO by CH4 over Co-ZSM-5 catalysts

et al. 2006

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The surface coverage analysis derived from two formal steady-state kinetic models is compared to values directly obtained from steady-state isotopic transient analysis (SSITKA) for the selective catalytic reduction (SCR) of NO by CH 4 over Co-ZSM-5 catalysts. It is shown that the most abundant reacting intermediates are NO x adspecies, though no clear differentiation between the various adspecies identified by DRIFT spectroscopy was achieved. Less numerous carbon containing adspecies were identified and quantified in the reacting system, essentially as methoxy species. Nitromethane-like intermediates remained undetectable due to a very rapid transformation into N 2 and CO 2 . On the basis of these converging kinetic analyses related to each elementary step of the SCR process, a microkinetic model can be derived, which allows describing transient operation, in view of a non steady-state application.

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“…The conversion of methane was 30% for the feed concentration considered (0.6%). More data is given in [13].…”

Section: Main Results Of the Ssitka Studymentioning

confidence: 99%

Section: Comparison Between Two Models a And Bmentioning

confidence: 99%

“…The various parameters were determined by minimizing root-mean-square deviation of experimental data from calculated ones [12,13].…”

Section: Numerical Analysis Of Ssitka Responsesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 96%

“…Changes in isotopic concentration after the 14 N 16 O/ 15 N 18 O switch under SCR conditions. Experimental data and modelled curves[13].…”

mentioning

confidence: 99%

See 3 more Smart Citations

Can isotopic transient and formal steady-state kinetics lead to a converging surface chemistry analysis? Case study on the selective reduction of NO by CH4 over Co-ZSM-5 catalysts

et al. 2006

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Mass Spectrometry in the SSITKA Studies

Пинаева

Sadovskaya

Suknev

et al. 2012

Mass Spectrometry Handbook

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Transient Catalytic Studies

Hinrichsen

2008

Handbook of Heterogeneous Catalysis

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The Importance of Transient Catalytic StudiesThe concept of using transient operations dates back to the late 1930s and the preliminary investigations conducted by Wagner and Hauffe [1,2]. Later, during the 1960s, Tamaru contributed substantially to this field in heterogeneous catalysis, in particular, by the use of the method of transient response [3] and by introducing the isotopic labeling technique [4]. Since then, transient methods have become standard tools for unraveling heterogeneously catalyzed reactions; for details, see the reviews in Refs. [5][6][7][8][9][10], monographs [11,12], and a special edition of Applied Catalysis [13]. The reasons for the wide application of transient methods are manifold. In chemical reactions, generally speaking, if the rate (rate equation, rate constant, and activation energy) of each of the elementary steps which comprise the overall reaction is known, the (micro)kinetics of the overall reaction may be understood. To take a simple example, in the reaction between hydrogen and bromine, the kinetics of the overall reaction follows a rather complicated rate law:However, if all the elementary reactions in the overall reaction are known, the kinetic behavior of the overall reaction may be explained on the basis of the rate constants, and the activation energies of the forward and backward reactions of the following elementary steps:In the case of such gas-phase reactions, the rate constants and activation energies of each of the elementary steps are independent of the concentration of reactants, reaction products, and reaction intermediates. This approximately also holds for reactions in solution.In the case of heterogeneously catalyzed reactions, the properties of the catalyst depend upon the concentrations of reactants, reaction intermediates, reaction products and, in some cases, spectator species that do not participate in the reaction path but which are chemisorbed on the catalyst surface. Furthermore, in many cases surface restructuring may occur along with the adsorption, and this results in marked changes in the reactivity of the surface. Consequently, even if the catalyst surface is kept in a well-defined state at the outset, as examined ex situ using a variety of spectroscopic techniques, it can be markedly different during the progress of reaction, and especially under industrially relevant reaction conditions. For example, in the case of oxide catalysts the extent of oxidation of the catalyst surface during the redox reaction is also influenced by the relative ratio of the rates of reduction and oxidation. This results in prominent changes in the properties of catalyst surfaces, depending upon the relative concentration of the reactants and the reaction temperature. In the case of acid catalysts, the acidity of the working catalyst surface (which should be associated with the catalytic activity) is that under the reaction conditions, and not that under the conditions far from those prevailing in the actual reaction.In the case of heterogeneous catalysis the rate co...

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Mechanism and Kinetics of the Selective NO Reduction over Co-ZSM-5 Studied by the SSITKA Technique

Cited by 23 publications

References 21 publications

Can isotopic transient and formal steady-state kinetics lead to a converging surface chemistry analysis? Case study on the selective reduction of NO by CH4 over Co-ZSM-5 catalysts

Can isotopic transient and formal steady-state kinetics lead to a converging surface chemistry analysis? Case study on the selective reduction of NO by CH4 over Co-ZSM-5 catalysts

Mass Spectrometry in the SSITKA Studies

Transient Catalytic Studies

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