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
Kinetic modelling
DFT
Methane oxidation
Palladium
Author
Carl-Robert Florén
Competence Centre for Catalysis (KCK)
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Maxime van den Bossche
Competence Centre for Catalysis (KCK)
Chalmers, Physics, Chemical Physics
Derek Creaser
Chalmers, Chemistry and Chemical Engineering, Chemical Technology
Competence Centre for Catalysis (KCK)
Henrik Grönbeck
Chalmers, Physics, Chemical Physics
Competence Centre for Catalysis (KCK)
Per-Anders Carlsson
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Competence Centre for Catalysis (KCK)
Heikki Korpi
Wärtsilä Finland
Magnus Skoglundh
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Competence Centre for Catalysis (KCK)
Catalysis Science and Technology
2044-4753 (ISSN) 2044-4761 (eISSN)
Vol. 8 2 508-520Competence Centre for Catalysis
Wärtsilä Finland, 2014-01-01 -- 2017-12-31.
Chalmers, 2014-01-01 -- 2017-12-31.
Volvo Group, 2014-01-01 -- 2017-12-31.
Haldor Topsoe, 2014-01-01 -- 2017-12-31.
Swedish Energy Agency (22490-3), 2014-01-01 -- 2017-12-31.
Scania CV AB, 2014-01-01 -- 2017-12-31.
Volvo Cars, 2014-01-01 -- 2017-12-31.
ECAPS AB, 2014-01-01 -- 2017-12-31.
Driving Forces
Sustainable development
Innovation and entrepreneurship
Areas of Advance
Nanoscience and Nanotechnology
Transport
Energy
Materials Science
Subject Categories
Physical Chemistry
Atom and Molecular Physics and Optics
Materials Chemistry
Roots
Basic sciences
Infrastructure
C3SE (Chalmers Centre for Computational Science and Engineering)
DOI
10.1039/c7cy02135f