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
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
收藏
页码:812 / 816
页数:5
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