title: Isothermal Cyclic Conversion of Methane into Methanol over Copper-Exchanged Zeolite at Low Temperature.
abstract: Direct partial oxidation of methane into methanol is a cornerstone of catalysis. The stepped conversion of methane into methanol currently involves activation at high temperature and reaction with methane at decreased temperature, which limits applicability of the technique. The first implementation of copper-containing zeolites in the production of methanol directly from methane is reported, using molecular oxygen under isothermal conditions at 200 °C. Copper-exchanged zeolite is activated with oxygen, reacts with methane, and is subsequently extracted with steam in a repeated cyclic process. Methanol yield increases with methane pressure, enabling reactivity with less reactive oxidized copper species. It is possible to produce methanol over catalysts that were inactive in prior state of the art systems. Characterization of the activated catalyst at low temperature revealed that the active sites are small clusters of copper, and not necessarily di- or tricopper sites, indicating that catalysts can be designed with greater flexibility than formerly proposed.
authors.affiliation: Institute for Chemistry and Bioengineering, HCI E 127, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland.|Paul Scherrer Institut, 5232, Villigen, Switzerland.
authors.forename: Patrick
authors.initials: P
authors.lastname: Tomkins
authors.affiliation: Institute for Chemistry and Bioengineering, HCI E 127, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland.|Paul Scherrer Institut, 5232, Villigen, Switzerland.
authors.forename: Ali
authors.initials: A
authors.lastname: Mansouri
authors.affiliation: Institute for Chemistry and Bioengineering, HCI E 127, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland.|Paul Scherrer Institut, 5232, Villigen, Switzerland.
authors.forename: Selmi E
authors.initials: SE
authors.lastname: Bozbag
authors.affiliation: Institute for Chemistry and Bioengineering, HCI E 127, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland.
authors.forename: Frank
authors.initials: F
authors.lastname: Krumeich
authors.affiliation: Institute for Chemistry and Bioengineering, HCI E 127, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland.|Paul Scherrer Institut, 5232, Villigen, Switzerland.
authors.forename: Min Bum
authors.initials: MB
authors.lastname: Park
authors.affiliation: Institute for Chemistry and Bioengineering, HCI E 127, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland.|Paul Scherrer Institut, 5232, Villigen, Switzerland.
authors.forename: Evalyn Mae C
authors.initials: EM
authors.lastname: Alayon
authors.affiliation: Paul Scherrer Institut, 5232, Villigen, Switzerland.
authors.forename: Marco
authors.initials: M
authors.lastname: Ranocchiari
authors.affiliation: Institute for Chemistry and Bioengineering, HCI E 127, Vladimir-Prelog-Weg 1, 8093, Zürich, Switzerland. Jeroen.vanbokhoven@psi.ch.|Paul Scherrer Institut, 5232, Villigen, Switzerland. Jeroen.vanbokhoven@psi.ch.
authors.forename: Jeroen A
authors.initials: JA
authors.lastname: van Bokhoven
keywords: copper zeolites; isothermal reaction; methane; methanol; partial oxidation