Kinetics investigation of NO plus CO reaction on La-Sr-Mn-O perovskite-type mixed oxides

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Συγγραφείς

Leontiou, A. A.
Ladavos, A. K.
Armatas, G. S.
Trikalitis, P. N.
Pomonis, P. J.

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Elsevier

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peer reviewed

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Όνομα περιοδικού

Applied Catalysis a-General

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Περιγραφή

Substituted perovskite-type mixed oxides of the general formula La1-xSrx(Mn-III/Mn-IV)O3+/-delta prepared by the nitrate method were examined by X-ray diffractometry (XRD) and the diffraction data were analyzed using the Rietveld refinement method. The amount of desorbed oxygen from the samples when heating in a He atmosphere was estimated with thermogravimetric O-2/temperature programmed desorption experiments while the amount of Mn-III and Mn-IV in the samples was determined iodometrically. The substitution of La3+ by Sr2+ leads to a gradual increase of Mn-IV in the solids and to the transition from an oxygen excess state to an oxygen deficient one. The samples were checked as catalysts for the reaction NO + CO --> products in a lab-scale plug-flow reactor between 220 and 560degreesC. The reaction rate profiles were simulated using a relationship of the form R = omega(1)R(low T) + omega(2)R(high) (T), where omega(1), omega(2) the weighing coefficients for the corresponding R at low R-low T and high temperatures R-high (T). From the fitting data the true activation energies E-1 and E-2 were estimated for R-low T and R-high T as well as the heats of adsorption DeltaH(ads(NO)) and AH(ads(CO)) for the NO and CO species. Finally, the values of E-app/low T estimated from typical Arrhenius plots ln R = f(1/T) at the low temperature region are in reasonable agreement with the difference E-1 - DeltaH(ads(NO)), a fact validating the results of simulation/fitting and indicating its usefulness for describing the reaction rates and estimating the kinetic and thermodynamic parameters controlling them. This methodology of simulation provides easily kinetic (activation energies) as well as thermodynamic (heats of adsorption) parameters which otherwise would necessitate differentiated experimental set-ups. (C) 2003 Elsevier B.V. All rights reserved.

Περιγραφή

Λέξεις-κλειδιά

perovskites, la-sr-mn-o, rietveld, no plus co reaction, kinetics, carbon-monoxide, catalytic-properties, defect structure, doped lamno3, nitric-oxide, reduction, oxygen, nonstoichiometry, combustion, methane

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<Go to ISI>://000221551600012
http://ac.els-cdn.com/S0926860X03010640/1-s2.0-S0926860X03010640-main.pdf?_tid=25aab3e9c8c928b2950fe3c55b6995d2&acdnat=1333036470_29c78726e6d87e06c925016833c31766

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en

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Γενική Περιγραφή / Σχόλια

Ίδρυμα και Σχολή/Τμήμα του υποβάλλοντος

Πανεπιστήμιο Ιωαννίνων. Σχολή Θετικών Επιστημών. Τμήμα Χημείας

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