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

被引：61

作者：

Meyet, Jordan ^{[1
]}

Searles, Keith ^{[1
]}

Newton, Mark A. ^{[1
]}

Worle, Michael ^{[1
]}

van Bavel, Alexander P. ^{[2
]}

Horton, Andrew D. ^{[2
]}

van Bokhoven, Jeroen A. ^{[1
,3
]}

Coperet, Christophe ^{[1
]}

机构：

[1] Swiss Fed Inst Technol, Dept Chem & Appl Biosci, Vladimir Prelog Weg 1-5, CH-8093 Zurich, Switzerland

[2] Shell Global Solut Int BV, Grasweg 31, NL-1031 HW Amsterdam, Netherlands

[3] Paul Scherrer Inst, Lab Catalysis & Sustainable Chem, CH-5232 Villigen, Switzerland

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2019年 / 58卷 / 29期

关键词：

alumina; C -H activation; copper; methane; methanol; ACTIVE-SITE; OXIDATION; CU; SURFACE; CU-ZSM-5; REACTIVITY; MORDENITE; STABILITY; CHEMISTRY; CLUSTERS;

D O I：

10.1002/anie.201903802

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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.

引用

页码：9841 / 9845

页数：5

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