Multiscale modelling of total pressure effects on complete methane oxidation over Pd/Al2O3
Licentiatavhandling, 2018

The models used in heterogeneous catalysis are becoming more advanced and the literature shows an increased interest in incorporating the atomistic scale into microkinetics. Coupling kinetics based on first-principles calculations to macroscopic effects can pave the way towards more comprehensive modelling methods and to tailored catalyst designs. The theme of this thesis is to coupling a reaction model based on first-principles to mass and heat transport and develop a multiscale reactor model for complete methane oxidation. The multiscale model is used to determine if the activity of an alumina supported palladium catalyst can be enhanced by increasing the reaction total pressure. First, a 1D porous catalyst model is developed where the kinetics and mass and heat transport is discussed for complete methane oxidation over Pd/Al2O3 for a simulated exhaust gas. It is shown that the catalyst performance can be enhanced by increasing the total pressure. However, the positive effect is constrained by a high coverage of the hindering surface species bicarbonates, adsorbed water and hydroxyl groups originating from the water and carbon dioxide in the bulk gas. The reaction controlling phenomena are identified for a range of temperatures and total pressures. Next, a 2D multiscale reactor model is developed to predict methane conversions. The conversion can be in- creased if the temperature is sufficiently high to overcome the desorption barriers of surface species hindering dissociative methane adsorption. The effects of total pressure on surface kinetics and mass and heat transport are discussed.

palladium oxide

mass and heat transport

multiscale modelling

reactor modelling

methane oxidation

first-principles calculations

Seminarierum 10:an, Kemigården 4


Carl-Robert Florén

Chalmers, Kemi och kemiteknik, Tillämpad kemi

Modelling complete methane oxidation over palladium oxide in a porous catalyst using first-principles surface kinetics

Catalysis Science and Technology,; Vol. 8(2018)p. 508-520

Artikel i vetenskaplig tidskrift

Carl-Robert Florén, Per-Anders Carlsson, Derek Creaser, Henrik Grönbeck, Magnus Skoglundh - Multiscale reactor modelling of total pressure effects for complete methane oxidation over Pd/Al2O3


Hållbar utveckling


Kemiska processer

Annan kemiteknik


C3SE (Chalmers Centre for Computational Science and Engineering)





Seminarierum 10:an, Kemigården 4

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