Catalysis of Metal Nanoclusters Synthesized in Porous Templates

目前的研究课题是在分子筛和介孔二氧化硅等微/介孔材料的有序纳米空间中模板合成新型金属纳米团簇，以及利用金属纳米团簇与多孔材料之间的协同效应进行新型分子转化的创新。我们发现介孔二氧化硅的介孔直径对Pt纳米颗粒催化CO在过量H2中PROX（优先氧化）反应活性的影响。在孔径为4.0 nm的介孔二氧化硅中，Pt纳米颗粒的催化活性最高。一些机理研究表明介孔二氧化硅不仅提供介孔空间，而且还表现出与金属物种协同的催化功能。我们还开发了选择性修饰介孔二氧化硅表面硅醇基的方法。制备了选择性外表面硅化的介孔二氧化硅，并对其进行了表征。研究了铜在其内表面固定化后在苯酚衍生物氧化聚合中的催化应用。

The present research topics are the template synthesis of novel metal nanoclusters in ordered nano-space of micro/meso materials such as zeolite and mesoporous silica and the innovation of novel molecular transformation by using a concerted effect between the metal nanoclusters and the porous materials. We found the dependence of mesopore diameter of mesoporous silica on the catalytic activity in Pt nanoparticles-catalyzed PROX(Preferential Oxidation)reaction of CO in excess H2. Pt nanoparticles in mesoporous silica with pore diameter of 4.0 nm show the highest catalytic activity than those with other pore diameters. Several mechanistic studies suggest that the mesoporous silica does not simply provide the mesospace but also exhibits concerted catalytic functions with the metal species. We also developed the methods for selective modification of surface silanol groups on mesoporous silica. The mesoporous silica silylated selectively on its external surface was prepared and characterized in detail. After immobilization of Cu species on its internal surface, catalytic application in oxidative polymerization of a phenol derivative was examined.