We have presented new amino-NHC Ni-Al complex mediated para C-H bond activation for pyridine and quinolin, and isolated for the first time the intermediate structure of a bimetallic eta(2),eta(1)-pyridine nickel aluminum complex prior to its C-H activation, which serves as key evidence for bimetallic catalysis.

We have successfully expanded the library of amino-NHCs with varying substituents on the amine group, leading to insight about the instability of NHCs arising from the intermolecular interaction of the dangling amine side-arm. However, the pendant amine plays an important role with respect to the catalytic process, resuscitating the catalytic activity of unsaturated NHC's through a synergistic effect invoked by the secondary amine. This proof of concept allows us to expand the spectrum of catalysis to C-C, as well as C-B bond formation.