Ligand Modification of Cyclometalated Ruthenium Complexes in the Aerobic Oxidative Dehydrogenation of Imidazolines

被引：15

作者：

Aiki, Shota ^{[1
]}

Kijima, Yuhei ^{[1
]}

Kuwabara, Junpei ^{[1
]}

Taketoshi, Ayako ^{[1
,2
]}

Koizumi, Take-aki ^{[3
]}

Akine, Shigehisa ^{[1
]}

Kanbara, Takaki ^{[1
]}

机构：

[1] Univ Tsukuba, Grad Sch Pure & Appl Sci, Tsukuba Res Ctr Interdisciplinary Mat Sci TIMS, Tsukuba, Ibaraki 3058573, Japan

[2] Tokyo Metropolitan Univ, Grad Sch Urban Environm Sci, Dept Appl Chem, Hachioji, Tokyo 1920397, Japan

[3] Tokyo Inst Technol, Chem Resources Lab, Midori Ku, Yokohama, Kanagawa 2268503, Japan

来源：

ACS CATALYSIS | 2013年 / 3卷 / 05期

关键词：

cyclometalated complex; ruthenium; homogeneous catalyst; dehydrogenation; aerobic oxidation; CHEMOSELECTIVE DEHYDROGENATION; 2-SUBSTITUTED IMIDAZOLINES; CATALYZED OXIDATION; METAL-CATALYSTS; ALCOHOLS; EFFICIENT; 2-IMIDAZOLINES; ALDEHYDES;

D O I：

10.1021/cs300811w

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

New cyclometalated ruthenium(III) complexes bearing 2-phenylpyridine derivatives were synthesized and characterized. Chemical, modification of the cyclometalating ligand affected its sigma-donor character and resulted in regulation of the redox potential of the ruthenium metal center; which was elucidated by-X-ray crystallography and cyclic voltammetry., The increase in the electron-donating ability of the cyclometalating ligand improved the catalytic activity of the ruthenium complexes in the aerobic oxidative dehydrogenation of 2-pherxylimidazoline, and enabled the catalytic dehydrogenation of 2-phenylimidazoline in air at room temperature. The effect of the ligand structure on the catalytic activity was also elucidated by density functional theory (DFT) calculations and titration experiments.

引用

页码：812 / 816

页数：5

共 52 条

[11] Efficient ruthenium-catalyzed aerobic oxidation of alcohols using a biomimetic coupled catalytic system [J].