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.

Catalytic oxidation

Kinetic modelling

DFT

Methane oxidation

Palladium

Författare

Carl-Robert Florén

Kompetenscentrum katalys

Chalmers, Kemi och kemiteknik, Tillämpad kemi

Maxime van den Bossche

Kompetenscentrum katalys

Chalmers, Fysik, Kemisk fysik

Derek Creaser

Chalmers, Kemi och kemiteknik, Kemiteknik

Kompetenscentrum katalys

Henrik Grönbeck

Chalmers, Fysik, Kemisk fysik

Kompetenscentrum katalys

Per-Anders Carlsson

Chalmers, Kemi och kemiteknik, Tillämpad kemi

Kompetenscentrum katalys

Heikki Korpi

Wärtsilä Finland

Magnus Skoglundh

Chalmers, Kemi och kemiteknik, Tillämpad kemi

Kompetenscentrum katalys

Catalysis Science and Technology

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

Vol. 8 2 508-520

Kompetenscentrum katalys KCK

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.

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

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

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

Energimyndigheten (22490-3), 2014-01-01 -- 2017-12-31.

Drivkrafter

Hållbar utveckling

Innovation och entreprenörskap

Styrkeområden

Nanovetenskap och nanoteknik (SO 2010-2017, EI 2018-)

Transport

Energi

Materialvetenskap

Ämneskategorier

Fysikalisk kemi

Atom- och molekylfysik och optik

Materialkemi

Fundament

Grundläggande vetenskaper

Infrastruktur

C3SE (Chalmers Centre for Computational Science and Engineering)

DOI

10.1039/c7cy02135f

Mer information

Senast uppdaterat

2022-04-05