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The 2006-2007 Beckman Scholars: Olga Leonidovna Dykhno
Beckman research project in the Willson Group: Download a copy of Olga's Research report, entitled "Toward the development of dynamic polymer catalysts".
Catalyst separation and recovery remain an important fundamental challenge in homogeneous metal-mediated reactions. As a result, extensive effort has been directed toward the pursuit of methods that balance catalyst recovery/reusability with activity and performance. Current approaches involve attachment of macromolecular materials, fluorous chains and other solubility-defining groups to the catalyst (or an appropriate precursor). While these concepts have had some success, they each suffer from mass transport issues and generally require biphasic media which necessitates significant amounts of solvent to effect quantitative precipitation. Clearly, a catalyst system that utilizes only one solvent and allows for quantitative recovery would provide an indispensable tool in metal-mediated synthetic reactions. Ultimately, this will lead to a significant reduction in purification costs and processes as well as a "greener" approach to metal-mediated catalysis. The aim of this research proposal is to utilize main chain organometallic polymers as recyclable polymer catalysts. The application of main-chain organometallic macromolecules in the area of metal-mediated catalysis is largely untapped. The paucity of examples is primarily because metal binding in the main-chain is either too labile (and thus depolymerization ensues spontaneously upon dissolution) or is saturated with ligands which leaves no open coordination modes for productive catalysis. We have recently discovered a new class organometallic polymers is that display the right balance between dynamic behavior (reversible depolymerization) and fidelity (structural integrity). These preliminary results open a new door for catalysts that integrate the high activities inherent to discrete (homogenous) complexes with the tunable, stimulus-responsive solubility characteristics of (heterogeneous) macromolecular materials. These are considerable advantages and can be expected to significantly impact the field of catalysis, especially in terms of catalyst recovery and reusability. |
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Created and maintained by Ruth Shear. Comments to author at DrRuth@mail.utexas.edu Created Mon Mar 9th 2004. Last modified Mon, Mar 16, 2015. |