Multifunctional reactive intermediates: preparation, characterization, reactivity and catalysis

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One of the prime elements for advancing chemical synthesis is the preparation, characterization, and control of multi-functional reactive intermediates. Currently, standard chemical technology typically employs mono- functional reactive species (organometallics, radicals, carbenes, cations, anions, etc.) and this seriously hampers the rapid construction of complex structures. Hence, most total syntheses involve a large number of steps and consequently are neither atom / mass nor energy economic. Despite the tremendous progress in this area, a much larger panel of reactions and especially reagents achieving a significant increase in structural complexity per chemical step is necessary. In this proposal five groups with diverse expertise have teamed together to prepare and study a variety of multi- functional reagents and reactive species that are possible intermediates in important synthetic transformations. Emphasis is on main group element reagents and reactive intermediates spanning from di- and tri- metallo hydrocarbons and silanes, to functionalized radicals and carbenes, to the analogous silicon-based intermediates, to oxenoids and nitrenoids and to transition metal functionalized reagents. The proposed research combines synthesis, mechanistic studies and the isolation of reactive intermediates in inert matrix and their spectroscopic characterization. It combines experiment and theoretical calculations which will provide additional insights into the nature of the many new reactive species which we plan to study. Overall, we believe that this research will enrich chemistry with many new multifunctional reagents and reactive species providing new possibilities for efficient synthesis of complex molecules.