The CO oxidation pattern of a nanocomposite MnCeOx catalyst (M5C1; Mnat/Ceat, 5) in the range of 293-533 K (P, 1 atm) has been probed under a kinetic regime, varying reagent pressure (p0CO, 0.01-0.025 atm; λ0, 1), ratio (λ0, 0.25-4.0) and CO2 co-feeding (0.05-0.10 atm). Activity data indicate fractional orders on pCO (0.6 ± 0.1) and pO2 (0.4 ± 0.1), with an activation energy of 40 ± 3 kJ mol-1, and a negative kinetic effect of CO2 co-feeding due to competitive adsorption processes. Coupled with systematic evidence on the reactivity and mobility of catalyst oxygen and surface intermediates, kinetic data disclose a concerted redox mechanism of Langmuir-Hinshelwood type, which starts by abstraction of O-atoms from surface active MnIV centres (r.d.s.), and is sustained by adsorption of diatomic oxygen species on O-vacancies. The derivative and integral forms of the formal rate equation explain the empirical kinetics, predicting the activity pattern of the MnCeOx catalyst in the range of 293-533 K.

A definitive assessment of the CO oxidation pattern of a nanocomposite MnCeO: X catalyst

Arena, Francesco
Primo
Membro del Collaboration Group
;
Di Chio, Roberto
Secondo
;
Espro, Claudia;
2018-01-01

Abstract

The CO oxidation pattern of a nanocomposite MnCeOx catalyst (M5C1; Mnat/Ceat, 5) in the range of 293-533 K (P, 1 atm) has been probed under a kinetic regime, varying reagent pressure (p0CO, 0.01-0.025 atm; λ0, 1), ratio (λ0, 0.25-4.0) and CO2 co-feeding (0.05-0.10 atm). Activity data indicate fractional orders on pCO (0.6 ± 0.1) and pO2 (0.4 ± 0.1), with an activation energy of 40 ± 3 kJ mol-1, and a negative kinetic effect of CO2 co-feeding due to competitive adsorption processes. Coupled with systematic evidence on the reactivity and mobility of catalyst oxygen and surface intermediates, kinetic data disclose a concerted redox mechanism of Langmuir-Hinshelwood type, which starts by abstraction of O-atoms from surface active MnIV centres (r.d.s.), and is sustained by adsorption of diatomic oxygen species on O-vacancies. The derivative and integral forms of the formal rate equation explain the empirical kinetics, predicting the activity pattern of the MnCeOx catalyst in the range of 293-533 K.
2018
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11570/3131878
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