Monomeric Copper(II) Sites Supported on Alumina Selectively Convert Methane to Methanol

Jordan Meyet; Keith Searles; Mark A. Newton; Michael Wörle; Alexander P. van Bavel; Andrew D. Horton; Jeroen A. van Bokhoven; Christophe Copéret

doi:10.1002/anie.201903802

Monomeric Copper(II) Sites Supported on Alumina Selectively Convert Methane to Methanol

Jordan Meyet
, Keith Searles
, Mark A. Newton
, Michael Wörle
, Alexander P. van Bavel
, Andrew D. Horton
, Jeroen A. van Bokhoven
, Christophe Copéret

Materials Research Institute (MRI)

Research output: Contribution to journal › Article › peer-review

67 Scopus citations

Abstract

Monomeric Cu^II 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 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 CH₃OH 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 CH₃O- surface species, can occur on pairs of proximal monomeric Cu^II sites in a short reaction time.

Original language	English (US)
Pages (from-to)	9841-9845
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	58
Issue number	29
DOIs	https://doi.org/10.1002/anie.201903802
State	Published - Jul 15 2019

All Science Journal Classification (ASJC) codes

Catalysis
General Chemistry

Access to Document

10.1002/anie.201903802

Cite this

@article{bbcc0d3dab3048c5bdfe4b731b137329,

title = "Monomeric Copper(II) Sites Supported on Alumina Selectively Convert Methane to Methanol",

abstract = "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.",

author = "Jordan Meyet and Keith Searles and Newton, \{Mark A.\} and Michael W{\"o}rle and \{van Bavel\}, \{Alexander P.\} and Horton, \{Andrew D.\} and \{van Bokhoven\}, \{Jeroen A.\} and Christophe Cop{\'e}ret",

note = "Publisher Copyright: {\textcopyright} 2019 Wiley-VCH Verlag GmbH \& Co. KGaA, Weinheim",

year = "2019",

month = jul,

day = "15",

doi = "10.1002/anie.201903802",

language = "English (US)",

volume = "58",

pages = "9841--9845",

journal = "Angewandte Chemie - International Edition",

issn = "1433-7851",

publisher = "John Wiley and Sons Ltd",

number = "29",

}

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

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.

UR - https://www.scopus.com/pages/publications/85067350612

UR - https://www.scopus.com/pages/publications/85067350612#tab=citedBy

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 -

Monomeric Copper(II) Sites Supported on Alumina Selectively Convert Methane to Methanol

Abstract

All Science Journal Classification (ASJC) codes

Access to Document

Other files and links

Fingerprint

Cite this