Pincer-based ligands have recently emerged as highly modular, redox robust scaffolds amenable to further synthetic elaboration. To engage novel substrate activation pathways, multifunctionality can be introduced within the secondary coordination sphere environment of a pincer-derived ligand. Our lab has initiated efforts toward the development of a series of pincer-based ligand architectures that, when metalated, feature well-positioned Lewis/Br�nsted acids and bases within the secondary coordination sphere of a metal complex. These ligands incorporate highly rigid frameworks to minimize the reorganizational energy upon substrate binding, and the specific functional groups were selected to favorably interact with metal-bound substrates. This presentation will outline efforts toward understanding the role that polar Lewis and Br�nsted acid/base groups in the periphery of a metal's coordination primary sphere environment might play to facilitate the binding/activation of substrates. Particular emphasis will be placed on design criteria of the appended functionality as well as new ways by which metal-ligand cooperativity can be exploited for substrate activation.

Exploiting pendant functionality within a pincer framework for cooperative substrate activation

246th National Meeting (2013)

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