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Isothermal Cyclic Conversion of Methane into Methanol over Copper‐Exchanged Zeolite at Low Temperature
Authors:Patrick Tomkins  Ali Mansouri  Dr Selmi E Bozbag  Dr Frank Krumeich  Dr Min Bum Park  Dr Evalyn Mae C Alayon  Dr Marco Ranocchiari  Prof?Dr Jeroen A van?Bokhoven
Institution:1. Institute for Chemistry and Bioengineering, HCI E 127, Zürich, Switzerland;2. Paul Scherrer Institut, Villigen, Switzerland
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.
Keywords:copper zeolites  isothermal reaction  methane  methanol  partial oxidation
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