化学
单体
电子顺磁共振
铜
甲醇
选择性
红外光谱学
氧化还原
无机化学
光化学
催化作用
有机化学
核磁共振
物理
聚合物
作者
Jordan Meyet,Keith Searles,Mark A. Newton,Michael Wörle,Alexander P. van Bavel,Andrew D. Horton,Jeroen A. van Bokhoven,Christophe Copéret
标识
DOI:10.1002/anie.201903802
摘要
Abstract 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.
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