期刊
CHEMICAL SCIENCE
卷 13, 期 13, 页码 3894-3901出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1sc07102e
关键词
-
资金
- European Research Council [ERC AdG 692775]
- Feinberg Graduate School, Weizmann Institute of Science
This study demonstrates an efficient and selective ruthenium-catalyzed synthesis of primary amides from alcohols and ammonia, with no need for acceptors. The selectivity of this system is rationalized through density functional theory calculations.
The highly desirable synthesis of the widely-used primary amides directly from alcohols and ammonia via acceptorless dehydrogenative coupling represents a clean, atom-economical, sustainable process. Nevertheless, such a reaction has not been previously reported, and the existing catalytic systems instead generate other N-containing products, e.g., amines, imines and nitriles. Herein, we demonstrate an efficient and selective ruthenium-catalyzed synthesis of primary amides from alcohols and ammonia gas, accompanied by H-2 liberation. Various aliphatic and aromatic primary amides were synthesized in high yields, with no observable N-containing byproducts. The selectivity of this system toward primary amide formation is rationalized through density functional theory (DFT) calculations, which show that dehydrogenation of the hemiaminal intermediate into primary amide is energetically favored over its dehydration into imine.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据