Webster-Gardiner, Michael

The catalytic activation of C-H bonds and the subsequent functionalization of hydrocarbons into heteroatom containing products is an area of fundamental importance in chemistry. Three different iridium pincer complexes for C-H activation were synthesized, IrCl3NNN, IrCl3NNN methyl, IrCl3NNNN (NNN= bis-((benzoimidazol))amine), (NNNmethyl = bis-(benzoimidazol)methyl)amine), and (NNNN = tris-((benzoimidazol))amine). These complexes were analyzed for C-H activation between benzoic acid and KOD/D2O solutions. We found that the C-H activation did not proceed catalytically. Also iron containing derivatives containing similar ligand motifs were synthesized , FeCl3NNNN, FeCl3IPI, FeCl3BPB, FeCl3BPB-OH (IPI = 2,6-diimidizoylpyridine, BPB = 2,6-dibenzoimidizoylpyridine, BPB-OH = 4-hydoxy-2,6,dibenzoimidizoylpyridine) and studied for their reactivity towards C-H bonds, O2 and N2 in aqueous basic media. The iron complexes were analyzed for the possibility of using them as O-atom or N-atom transfer reagents for hydrocarbon oxidation. Preliminary results suggest that upon reduction the iron complexes are capable of direct reaction with O2 and N2.