The utility of frustrated Lewis acid/base chemistry has recently become highly popularized. While metal-free systems have significantly advanced strategies for small-molecule transformations, further redox transformations of substrate-FLP adducts are typically limited. Our lab has initiated efforts toward the development of a series of ligand architectures that, when metalated, position Lewis pairs within a metal's secondary coordination sphere. The appended Lewis pairs were selected to favorably interact with an appropriate metal-bound substrate to facilitate binding and redox transformations. This talk will outline efforts toward understanding the role that polar Lewis acid/base groups in the periphery of a metal's coordination sphere might play to facilitate substrate binding/activation. Particular emphasis will be placed on synthetic approaches and design strategies to generate systems with appended functionality, and their subsequent reactivity with small molecules. Furthermore, parallels between Lewis-pair appended transition metal systems with FLP chemistry will be described.

Putting the metal back in FLP chemistry: Transition metal complexes with appended Lewis acids and bases for cooperative reactivity

245th National Meeting (2013)

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