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 2 508-520Kompetenscentrum katalys KCK
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.
Energimyndigheten (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.
Drivkrafter
Hållbar utveckling
Innovation och entreprenörskap
Styrkeområden
Nanovetenskap och nanoteknik
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