Modelling complete methane oxidation over palladium oxide in a porous catalyst using first-principles surface kinetics
Artikel i vetenskaplig tidskrift, 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.

Methane oxidation

Kinetic modelling

Catalytic oxidation

Palladium

DFT

Författare

Carl-Robert Florén

Kompetenscentrum katalys (KCK)

Chalmers, Kemi och kemiteknik

Maxime van den Bossche

Chalmers, Fysik, Kemisk fysik

Kompetenscentrum katalys (KCK)

Derek Creaser

Chalmers, Kemi och kemiteknik

Kompetenscentrum katalys (KCK)

Henrik Grönbeck

Chalmers, Fysik, Kemisk fysik

Kompetenscentrum katalys (KCK)

Per-Anders Carlsson

Chalmers, Kemi och kemiteknik

Kompetenscentrum katalys (KCK)

Heikki Korpi

Wärtsilä Finland

Magnus Skoglundh

Chalmers, Kemi och kemiteknik

Kompetenscentrum katalys (KCK)

Catalysis Science and Technology

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

Vol. 8 508-520

Kompetenscentrum katalys KCK

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

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

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

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

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

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

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

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

Drivkrafter

Hållbar utveckling

Innovation och entreprenörskap

Styrkeområden

Nanovetenskap och nanoteknik

Transport

Energi

Materialvetenskap

Ämneskategorier

Fysikalisk kemi

Kemiska processer

Atom- och molekylfysik och optik

Materialkemi

Annan kemiteknik

Teoretisk kemi

Fundament

Grundläggande vetenskaper

Infrastruktur

C3SE (Chalmers Centre for Computational Science and Engineering)

DOI

10.1039/c7cy02135f

Mer information

Senast uppdaterat

2018-10-27