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Isothermal Cyclic Conversion of Methane into Methanol over Copper‐Exchanged Zeolite at Low Temperature
Author(s) -
Tomkins Patrick,
Mansouri Ali,
Bozbag Selmi E.,
Krumeich Frank,
Park Min Bum,
Alayon Evalyn Mae C.,
Ranocchiari Marco,
van Bokhoven Jeroen A.
Publication year - 2016
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201511065
Subject(s) - methane , methanol , catalysis , zeolite , copper , chemistry , inorganic chemistry , isothermal process , anaerobic oxidation of methane , reactivity (psychology) , partial oxidation , oxidative coupling of methane , yield (engineering) , organic chemistry , materials science , metallurgy , thermodynamics , medicine , physics , alternative medicine , pathology
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.