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去甲基尼古丁在含水二甲基亞礬溶劑中催化曼尼希反應之理論研究
Thesis

去甲基尼古丁在含水二甲基亞礬溶劑中催化曼尼希反應之理論研究

楊昇哲
Masters, 國立清華大學, 化學系
2010

Abstract

密度泛函理論 曼尼希反應 去甲基尼古丁 有機催化 density functional theory Mannich reaction nornicotine catalyst water
The nornicotine catalyzed Mannich reaction and its mechanism are analyzed with quantum chemical calculations by M06-2X/6-31++G(d,p) method and the polarizable continuum model (PCM) for the solvent effect of dimethyl sulfoxide. The Mannich reaction with nornicotine as a catalyst can be separated into three steps. First, the nornicotine-derived enamine is generated from nornicotine and a ketone with the aid of a water molecule. Second, the nornicotine-derived enamine forms a C-C bond with the imine to produce a chiral intermediate with the assistance of a water molecule. There are four possible stereo-control paths and the analysis suggests that nornicotine as a catalyst favors the S- over R-Mannich product. Third, water catalyzes the release of the original nornicotine catalyst from the Mannich product. The calculation indicates that water is a key element in the proposed mechanism and that nornicotine can catalyze the Mannich reaction in wet solvents or even pure water.

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