Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 55, Issue 18, Pages 5467-5471Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201511065
Keywords
copper zeolites; isothermal reaction; methane; methanol; partial oxidation
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Funding
- Turkish Scientific and Technological Research Council (TUBITAK) [2219]
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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 degrees 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.
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