title: Ketene as a Reaction Intermediate in the Carbonylation of Dimethyl Ether to Methyl Acetate over Mordenite.
abstract: Unprecedented insight into the carbonylation of dimethyl ether over Mordenite is provided through the identification of ketene (CH2CO) as a reaction intermediate. The formation of ketene is predicted by detailed DFT calculations and verified experimentally by the observation of doubly deuterated acetic acid (CH2DCOOD), when D2O is introduced in the feed during the carbonylation reaction.
authors.affiliation: Department of Chemical and Biochemical Engineering, Technical University of Denmark, Building 229, 2800 Kgs. Lyngby (Denmark).
authors.forename: Dominik B
authors.initials: DB
authors.lastname: Rasmussen
authors.affiliation: Department of Chemical and Biochemical Engineering, Technical University of Denmark, Building 229, 2800 Kgs. Lyngby (Denmark). jmc@kt.dtu.dk.
authors.forename: Jakob M
authors.initials: JM
authors.lastname: Christensen
authors.affiliation: Haldor Topsøe Research Laboratories, Nymøllevej 55, 2800 Kgs. Lyngby (Denmark).
authors.forename: Burcin
authors.initials: B
authors.lastname: Temel
authors.affiliation: SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025 (USA).
authors.forename: Felix
authors.initials: F
authors.lastname: Studt
authors.affiliation: Haldor Topsøe Research Laboratories, Nymøllevej 55, 2800 Kgs. Lyngby (Denmark).
authors.forename: Poul Georg
authors.initials: PG
authors.lastname: Moses
authors.affiliation: Department of Physics, Technical University of Denmark, Building 307, 2800 Kgs. Lyngby (Denmark).
authors.forename: Jan
authors.initials: J
authors.lastname: Rossmeisl
authors.affiliation: Center for Catalysis and Sustainable Chemistry, Department of Chemistry, Technical University of Denmark, Building 207, 2800 Kgs. Lyngby (Denmark).
authors.forename: Anders
authors.initials: A
authors.lastname: Riisager
authors.affiliation: Department of Chemical and Biochemical Engineering, Technical University of Denmark, Building 229, 2800 Kgs. Lyngby (Denmark). aj@kt.dtu.dk.
authors.forename: Anker D
authors.initials: AD
authors.lastname: Jensen
keywords: carbonylation; density functional calculations; heterogeneous catalysis; reaction mechanisms; zeolites