We propose that PA coordination to Fe in a chelating fashion and reduction of Fe(+3) to Fe(+2) (by t BuOOH) initiates the catalytic cycle via formation of complex 34. Coordination of one amine molecule and oxidation by PhCO 3 t Bu to the Fe(+4) oxo intermediate 35 is then followed by a radical rebound step, resulting in α-C-H hydroxylation of the coordinated amine to yield Fe(+2) intermediate 36. Dissociation of the hemiaminal is then followed by the formation of an iminium intermediate, which in turn reacts with the cyanide nucleophile that is solubilized by 18-crown-6 to obtain product 37. Coordination of hydroxide and another ligand L to Fe completes the catalytic cycle and reforms 34.