Experiments and DFT Computations Combine to Decipher Fe- Catalyzed Amidine Synthesis through Nitrene Transfer and Nitrile Insertion

The development of multicomponent reactions (MCR) is the prefered eco-compatible approach to sophisticated molecules of pharmaceutical interest, such as amidines. We elaborated a new MCR to amidines which produces them in good yields under mild conditions through an Fe-catalyzed combination of a hydrocarbon, a nitrile, and a nitrene. We solved the mechanism of this reaction by developing an integrated combination of experiments and DFT calculations which provides a detailed description of all involved molecular events and an estimation of their energetic cost.