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醇-胺(氨)直接脱氢及氧化脱氢偶联生成酰胺具有原子经济性高和对环境友好等优点,因而受到广泛关注。研究发现,一些过渡金属钌及铑配合物、负载金及银纳米粒子、氧化锰分子筛(OMS-2)以及基于铜、铁化合物的催化体系在醇-胺(氨)直接脱氢或氧化脱氢偶联生成酰胺反应中显示出优良的催化性能。本文首先介绍了PNN-钌、NHC-钌配合物、铑配合物以及负载银原子簇催化的醇-胺(氨)直接脱氢偶联生成酰胺反应的研究进展,然后对负载纳米金粒子、氧化锰分子筛(OMS-2)以及基于铜、铁化合物的催化体系催化的不同氧化剂,包括分子氧、叔丁基过氧化氢以及分子碘氧化的氧化酰胺化反应进行了总结。对各催化剂或催化体系的适用范围和优缺点进行了分析,阐述了主要催化剂或催化体系的催化机理。此外,还对无过渡金属参与的醇-胺氧化酰胺化反应体系进行概述。最后,在总结现有成果的基础上指出了该领域的发展方向。
Alcohol - amine (ammonia) direct dehydrogenation and oxidative dehydrogenation coupled to produce amides with the advantages of high atom economy and environment-friendly, which attracted widespread attention. It has been found that some of the transition metal ruthenium and rhodium complexes, supported gold and silver nanoparticles, manganese oxide molecular sieve (OMS-2), and catalytic systems based on copper and iron compounds are directly dehydrogenated or oxidatively dehydrogenated Coupling to generate amide reaction shows excellent catalytic performance. In this paper, the progress of the direct dehydrogenation coupling of PNN-ruthenium, NHC-ruthenium complex, rhodium complex and alcohol-amine (ammonia) catalyzed by supported silver clusters to amide formation was introduced. Manganese molecular sieves (OMS-2) and the oxidative amidation reactions of different oxidants, including molecular oxygen, t-butyl hydroperoxide and molecular iodine catalyzed by catalytic systems based on copper and iron compounds were summarized. The application range, advantages and disadvantages of each catalyst or catalyst system are analyzed, and the catalytic mechanism of the main catalyst or catalyst system is expounded. In addition, the alcohol-amine amidation reaction system without transition metal is also summarized. Finally, on the basis of summarizing the existing achievements, we point out the development direction in this field.