Weakly coordinating anions (WCAs) are generally tailored to act as spectators with little or no function. Here we demonstrate the implementation of strongly coordinating dianionic carboranyl N-Heterocyclic Carbenes (NHCs) to create organometallic ate complexes of Au(I) that serve both as WCAs and functional catalysts. These organometallic WCAs can be utilized to form both heterobimetallic (Au(I)-/Ag(I)+) and organometallic/main group ion pairs (Au(I)-/(CPh3+ or SiEt3+). As the parent unfunctionalized dianionic carboranyl NHC complex is unstable in most solvents when paired with CPh3+, novel synthetic methodology was devised to create polyhalogenated carboranyl NHCs, which show superior stability towards electrophilic substitution and cyclometalation chemistry. Additionally, the WCAs containing polyhalogenated carboranyl NHCs are among the most active catalysts reported for the hydroamination of alkynes. This investigation has also produced the first examples of a pseudo-low coordinate Au(III) center with two cis accessible coordination sites and the first true dianionic carbene. These studies pave the way for the design of functional ion pairs that have the potential to participate in tandem or cooperative small molecule activation and catalysis.

Strongly coordinating ligands to create weakly coordinating yet functional anions

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.