介孔Mn_(0.5)Fe_(0.5)O_(x)颗粒的制备及其在醇胺氧化偶联反应中的应用

Preparation of Mesoporous Mn_(0.5)Fe_(0.5)O_(x) Particles and Their Application in the Oxidative Coupling Reaction of Alcohols with Amines

研发一种廉价、高效的催化剂以提高醇胺氧化偶联合成亚胺的催化活性具有重要意义。本文采用简单的共沉淀法制备了一系列锰铁双金属氧化物,并将其应用于苯甲醇和苯胺氧化偶联合成N-苄叉苯胺的催化反应,以及探索了不同的锰铁投料比对产物催化活性的影响。结果表明,锰铁投料比为1:1时的产物(Mn_(0.5)Fe_(0.5)O_(x))具有最佳的催化活性,其苯胺转化率为74.7%,N-苄叉苯胺的选择性和收率分别为99.9%和74.6%。通过多种表征发现,Mn_(0.5)Fe_(0.5)O_(x)具有丰富的介孔结构和表面吸附氧物种以及优异的氧化能力,因而展现出优异的催化活性。本文所制备的高活性催化剂在醇胺氧化偶联制备亚胺的方法中具有较大的应用潜力。

It is of great significance to develop an inexpensive and efficient catalyst to enhance the catalytic activity of oxidation coupling of alcohols with amines to imine.In this research,a series of manganese-iron bimetallic oxide catalysts have been prepared by a simple co-precipitation method,which were applied to the catalytic reaction of oxidation coupling of benzyl methanol with aniline to N-benzylideneaniline.The effects of different Fe/Mn feed ratios on the catalytic activity of the products have been explored.The Mn_(0.5)Fe_(0.5)O_(x) sample with a Fe/Mn feed ratio of 1:1 demonstrated the best catalytic activity,giving an aniline conversion rate of 74.7%,99.9%selectivity and 74.6%yield of N-benzylidene,respectively.Through a variety of characterizations,Mn_(0.5)Fe_(0.5)O_(x) exhibited rich mesoporous structure and surface adsorbed oxygen species,as well as excellent oxidation ability.The highefficiency catalyst synthesized in this work has great application potential in the preparation of imines by oxidation coupling of alcohols with amines.