Modelling complete methane oxidation over palladium oxide in a porous catalyst using first-principles surface kinetics
Journal article, 2018

A comprehensive model is developed for complete methane oxidation over supported palladium. The model is based on first-principles microkinetics and accounts for mass and heat transport in a porous catalytic layer. The turnover frequency (TOF) is simulated for wet exhaust gas compositions, exploring the effects of temperature and total pressure on the TOF. Three different temperature regimes are identified each with different dependency on the total pressure. The regimes originate from temperature and pressure dependent coverages of carbon dioxide and water, which are the most abundant surface species hindering methane dissociation at low temperatures. The TOF is controlled by surface kinetics below 400 °C whereas above 500 °C and up to 8 atm, internal mass transport is controlling. A combination of kinetics, external and internal mass transport controls the TOF at other reaction conditions. The physically meaningful model paves the way for extrapolation and optimization of catalyst design parameters for high catalytic efficiency.

Catalytic oxidation

DFT

Methane oxidation

Kinetic modelling

Palladium

Author

Carl-Robert Florén

Competence Centre for Catalysis (KCK)

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Applied Surface Chemistry

Maxime van den Bossche

Competence Centre for Catalysis (KCK)

Chalmers, Physics, Chemical Physics

Derek Creaser

Competence Centre for Catalysis (KCK)

Chalmers, Chemistry and Chemical Engineering, Chemical Technology, Forest Products and Chemical Engineering

Henrik Grönbeck

Competence Centre for Catalysis (KCK)

Chalmers, Physics, Chemical Physics

Per-Anders Carlsson

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Applied Surface Chemistry

Competence Centre for Catalysis (KCK)

Heikki Korpi

Wärtsilä Finland

Magnus Skoglundh

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Applied Surface Chemistry

Competence Centre for Catalysis (KCK)

Catalysis Science and Technology

2044-4753 (ISSN) 2044-4761 (eISSN)

Vol. 8 2 508-520

Competence Centre for Catalysis

Volvo Group, 2014-01-01 -- 2017-12-31.

Volvo Cars, 2014-01-01 -- 2017-12-31.

ECAPS AB, 2014-01-01 -- 2017-12-31.

Chalmers, 2014-01-01 -- 2017-12-31.

Wärtsilä Finland, 2014-01-01 -- 2017-12-31.

Scania CV AB, 2014-01-01 -- 2017-12-31.

Swedish Energy Agency, 2014-01-01 -- 2017-12-31.

Haldor Topsoe, 2014-01-01 -- 2017-12-31.

Driving Forces

Sustainable development

Innovation and entrepreneurship

Areas of Advance

Nanoscience and Nanotechnology (SO 2010-2017, EI 2018-)

Transport

Energy

Materials Science

Subject Categories

Physical Chemistry

Chemical Process Engineering

Atom and Molecular Physics and Optics

Materials Chemistry

Other Chemical Engineering

Theoretical Chemistry

Roots

Basic sciences

Infrastructure

C3SE (Chalmers Centre for Computational Science and Engineering)

DOI

10.1039/c7cy02135f

More information

Latest update

3/25/2021