Abhi Karkamkar1

1, Pacific Northwest National Laboratory, Richland, Washington, United States

We have synthesized stable homotopic, single-site catalysts supported on MCM-41 by a combination of sol-gel and surface organometallic chemistry (SOMC). We have demonstrated that a variety of metal atoms (Cu, Ru and Rh) can be anchored on these ligands. In addition to incorporation of single metal sites we have been able to incorporate multi-nuclear clusters of metals. We have devised and synthesized monomeric, dimeric, trimeric and tetrameric clusters that have been incorporated in high surface area mesoporous silica with high degree of control. Structural characterization of these catalytic materials has shown desirable properties such as high surface area, high degree of porosity and high thermal stability. We synthesized several versions of MCM-41-supported ligands and characterized them by multinuclear NMR, FTIR, and MS.
Here we present our progress in the area of synthesis of organo-functional hybrid catalysts that are promising towards the direct conversion of alkanes to alcohols. Synthetic analogues have provided some insight into the process of converting alkanes to alcohols with varying degree of control and success. Such hybrid solids are well defined at the molecular level and may allow a greater understanding and a more rational analysis of the structural relationship between reactants and products. We have synthesized Schiff-base functionalized organo-functional hybrid catalysts and then evaluated their activity towards oxidation of alkanes.