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Monomeric Copper(II) Sites Supported on Alumina Selectively Convert Methane to Methanol
Author(s) -
Meyet Jordan,
Searles Keith,
Newton Mark A.,
Wörle Michael,
van Bavel Alexander P.,
Horton Andrew D.,
van Bokhoven Jeroen A.,
Copéret Christophe
Publication year - 2019
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201903802
Subject(s) - chemistry , monomer , electron paramagnetic resonance , copper , selectivity , methanol , infrared spectroscopy , redox , photochemistry , inorganic chemistry , catalysis , organic chemistry , nuclear magnetic resonance , physics , polymer
Monomeric Cu II sites supported on alumina, prepared using surface organometallic chemistry, convert CH 4 to CH 3 OH selectively. This reaction takes place by formation of CH 3 O surface species with the concomitant reduction of two monomeric Cu II sites to Cu I , according to mass balance analysis, infrared, solid‐state nuclear magnetic resonance, X‐ray absorption, and electron paramagnetic resonance spectroscopy studies. This material contains a significant fraction of Cu active sites (22 %) and displays a selectivity for CH 3 OH exceeding 83 %, based on the number of electrons involved in the transformation. These alumina‐supported Cu II sites reveal that C−H bond activation, along with the formation of CH 3 O‐ surface species, can occur on pairs of proximal monomeric Cu II sites in a short reaction time.