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Low-temperature CO oxidation over a Pt/Al2O3 monolith catalyst investigated by step-response experiments and simulations

Per-Anders Carlsson (Institutionen för kemi- och bioteknik, Kemisk reaktionsteknik ; Kompetenscentrum katalys (KCK)) ; Magnus Skoglundh (Institutionen för kemi- och bioteknik, Teknisk ytkemi ; Kompetenscentrum katalys (KCK)) ; Peter Thormählen (Institutionen för teknisk fysik, Kemisk fysik ; Kompetenscentrum katalys (KCK)) ; Bengt Andersson (Institutionen för kemi- och bioteknik, Kemisk reaktionsteknik ; Kompetenscentrum katalys (KCK))
Topics in Catalysis (1022-5528). Vol. 30/31 (2004), 1-4, p. 375-381.
[Artikel, refereegranskad vetenskaplig]

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.

Nyckelord: cold-start, self-poisoning, low-temperature activity, step-response experiment, CO oxidation, catalytic ignition, catalytic extinction, mean-field modelling, simulations, Pt/Al2O3



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Denna post skapades 2006-08-28. Senast ändrad 2014-10-27.
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Institutioner (Chalmers)

Institutionen för kemi- och bioteknik, Kemisk reaktionsteknik (2005-2014)
Kompetenscentrum katalys (KCK)
Institutionen för kemi- och bioteknik, Teknisk ytkemi (2005-2014)
Institutionen för teknisk fysik, Kemisk fysik (1900-2015)

Ämnesområden

Energi
Materialvetenskap
Nanovetenskap och nanoteknik
Transport
Hållbar utveckling
Miljökemi
Kemiteknik

Chalmers infrastruktur

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