Reactivity Study of well-defined Heterogeneous Group IV Metal Complexes Prepared via SOMC

Peijie Hu, Jose Berger, Keith Searles

University of Florida

Surface organometallic chemistry (SOMC) is a methodology to generate well-defined heterogeneous catalysts. By applying molecular-level techniques and characterization methods on heterogeneous catalysts, structure of surface sites can be pictured and thus it becomes possible to establish structure-reactivity relationships facilitating understanding of reaction mechanisms and rational design of new catalysts.

Over the past decades, oxide supports have been a prevalent choice in this field owing to extensive investigation and a comprehensive understanding of their structures. Group IV metals (Ti, Zr, Hf) have been grafted on SiO₂ support and demonstrated activity towards hydrogenolysis, hydrogenation and polymerization reactions. We would like to present our work in an effort to elucidate the mechanisms and identify active sites through both semi-batch and flow reactions, in particular, arene hydrogenation and propane hydrogenolysis reactions.

At the meantime, the effect of support on the reactivity of these heterogeneous catalysts is also explored. Non-traditional supports, such as silicon nitride (Si₃N₄), are promising as a candidate for an alternate support. This poster will highlight our laboratory’s recent study on Si₃N₄ supported early transition metal complexes. The synthesis of Si₃N₄ as a support, including characterization and control of its surface functionalities, will be discussed.