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Importance of Methane Chemical Potential for Its Conversion to Methanol on Cu‐Exchanged Mordenite
Author(s) -
Zheng Jian,
Lee Insu,
Khramenkova Elena,
Wang Meng,
Peng Bo,
Gutiérrez Oliver Y.,
Fulton John L.,
Camaioni Donald M.,
Khare Rachit,
Jentys Andreas,
Haller Gary L.,
Pidko Evgeny A.,
SanchezSanchez Maricruz,
Lercher Johannes A.
Publication year - 2020
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.202000772
Subject(s) - mordenite , methanol , methane , zeolite , chemistry , stoichiometry , inorganic chemistry , desorption , yield (engineering) , catalysis , materials science , adsorption , organic chemistry , metallurgy
Copper‐oxo clusters exchanged in zeolite mordenite are active in the stoichiometric conversion of methane to methanol at low temperatures. Here, we show an unprecedented methanol yield per Cu of 0.6, with a 90–95 % selectivity, on a MOR solely containing [Cu 3 (μ‐O) 3 ] 2+ active sites. DFT calculations, spectroscopic characterization and kinetic analysis show that increasing the chemical potential of methane enables the utilization of two μ‐oxo bridge oxygen out of the three available in the tricopper‐oxo cluster structure. Methanol and methoxy groups are stabilized in parallel, leading to methanol desorption in the presence of water.