表面富锡MCM-41分子筛的表面金属有机化学制备及其对苯酚羟基化催化反应性能研究

Preparation of MCM-41 Richened Tin on the Surface by Surface Organometallic Chemistry and its Catalytic Performance for Hydroxylation of Phenol

采用SnBu4在MCM-41表面的接枝反应和后续处理制备出了一种只在表面含锡的MCM-41型介孔分子筛。通过与采用纳米SnO2和MCM-41机械混合法、SnCl4浸渍法、水热合成法等制备的具有相当硅锡比(Si/Sn≈100)的SnMCM-41分子筛进行结构和对苯酚羟基化反应催化性能的比较发现,由该法所得分子筛的水热稳定性明显提高,并在苯酚羟基化反应中表现出优良的催化活性、选择性和过氧化氢利用率。本文还详细考察了该催化剂对苯酚羟基化反应的最佳反应条件。

A mesoporous MCM-41 molecular sieve richened tin on the surface was prepared by a grafting reaction of SnBu4 on the surface of MCM-41 in vacuum followed by a treatment in flow of oxygen. Compared to SnMCM-41 with comparable ratio of Si/Sn(Si/Snapproximate to100) prepared by the mechanical commixture of nanometer SnO2 with MCM-41, the use of the impregnation of MCM-41 with SnCl4 solution as well as the hydrothermal synthesis route, the obtained sample had better hydrothermal stability and, presented better catalytic activity, higher selectivity of diphenol and higher chemical availability of H2O2 in hydroxylation reaction of the phenol. Some optimal conditions of the reaction were also investigated in the paper.