TY - JOUR
T1 - Monomeric Copper(II) Sites Supported on Alumina Selectively Convert Methane to Methanol
AU - Meyet, Jordan
AU - Searles, Keith
AU - Newton, Mark A.
AU - Wörle, Michael
AU - van Bavel, Alexander P.
AU - Horton, Andrew D.
AU - van Bokhoven, Jeroen A.
AU - Copéret, Christophe
N1 - Funding Information:
J.M. and M.A.N. thank Shell Global Solutions International B.V. for financial support. We acknowledge the European Synchrotron Radiation Facility, Grenoble, France, for synchrotron resources (beamline BM31; CH 5579) and we thank H. Emerich and D. Stoian for their assistance. We thank A. J. Knorpp and P. Sˇ ot for their help with XAS experiments, T. Margossian and F. Allouche for discussions, and A. Ashuiev for his help with EPR.
Publisher Copyright:
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2019/7/15
Y1 - 2019/7/15
N2 - Monomeric CuII sites supported on alumina, prepared using surface organometallic chemistry, convert CH4 to CH3OH selectively. This reaction takes place by formation of CH3O surface species with the concomitant reduction of two monomeric CuII sites to CuI, 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 CH3OH exceeding 83 %, based on the number of electrons involved in the transformation. These alumina-supported CuII sites reveal that C−H bond activation, along with the formation of CH3O- surface species, can occur on pairs of proximal monomeric CuII sites in a short reaction time.
AB - Monomeric CuII sites supported on alumina, prepared using surface organometallic chemistry, convert CH4 to CH3OH selectively. This reaction takes place by formation of CH3O surface species with the concomitant reduction of two monomeric CuII sites to CuI, 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 CH3OH exceeding 83 %, based on the number of electrons involved in the transformation. These alumina-supported CuII sites reveal that C−H bond activation, along with the formation of CH3O- surface species, can occur on pairs of proximal monomeric CuII sites in a short reaction time.
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U2 - 10.1002/anie.201903802
DO - 10.1002/anie.201903802
M3 - Article
C2 - 31069914
AN - SCOPUS:85067350612
SN - 1433-7851
VL - 58
SP - 9841
EP - 9845
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 29
ER -