Low-temperature CO oxidation over a Pt/Al2O3 monolith catalyst investigated by step-response experiments and simulations
Artikel i vetenskaplig tidskrift, 2004

The ignition–extinction processes for CO oxidation over a Pt/Al2O3 monolith catalyst have been studied by flow-reactor experiments and simulations. The study was performed by stepwise changes of the inlet O2 concentration ranging 0–20 vol% while the CO concentration and the inlet gas temperature were kept constant at 1.0 vol% and 423 K, respectively. Several features observed experimentally are qualitatively simulated with our model: (i) the ignition of the CO oxidation demands 8.0vol% O2 (ii) corresponding to a catalyst ignition temperature of 433 K (due to the exothermicity of the reaction) and (iii) occurs in the rear part of the monolith where (iv) a local reaction zone is formed which (v) moves towards the reactor inlet as a function of time on stream. Additionally, the simulations show first order kinetic phase transitions, i.e. rapid adsorbate concentration changes, where the catalyst surface is predominantly CO covered in the low reactive state and almost completely oxygen covered in the high reactive state. For the ignition process the kinetic phase transition occurs after the actual catalytic ignition. However, the extinction process is more difficult to simulate dynamically without changing the model parameters for O2 adsorption in the low and high reactive state, respectively. The influence of diffusion limitations and the role of formation of a less reactive Pt state under oxidising conditions is discussed.

step-response experiment

Pt/Al2O3

low-temperature activity

cold-start

catalytic ignition

self-poisoning

mean-field modelling

simulations

catalytic extinction

CO oxidation

Författare

Per-Anders Carlsson

Kompetenscentrum katalys (KCK)

Chalmers, Kemi- och bioteknik, Kemisk reaktionsteknik

Magnus Skoglundh

Chalmers, Kemi- och bioteknik, Teknisk ytkemi

Kompetenscentrum katalys (KCK)

Peter Thormählen

Chalmers, Teknisk fysik, Kemisk fysik

Kompetenscentrum katalys (KCK)

Bengt Andersson

Kompetenscentrum katalys (KCK)

Chalmers, Kemi- och bioteknik, Kemisk reaktionsteknik

Topics in Catalysis

1022-5528 (ISSN) 1572-9028 (eISSN)

Vol. 30/31 375-381

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