Exploring Low-Coordinate Aluminum-Based Lewis Acids for Small Molecule Activation

While there have been a significant number of publications in the field of frustrated Lewis pair chemistry, only a fraction employ aluminum-based Lewis acids. The research presented herein expands the scope of Lewis acids to include novel aluminum-based compounds.;N-heterocyclic carbene-stabilized three-coordinate aluminum cations were synthesized from the NHC-AlR3 adduct by abstraction of an R substituent from aluminum. These compounds were crystallographically characterized and exhibited solvent-dependent reactivity. Hydrogenation catalysis and radical reactivity were also explored experimentally and computationally.