Multiple Oxidative Dehydrogenative Functionalization of Arylacetaldehydes Using Molecular Oxygen as Oxidant Leading to 2‐Oxo‐acetamidines

A novel copper‐catalyzed, multiple oxidative dehydrogenative functionalization of arylacetaldehydes leading to 2‐oxo‐acetamidine compounds has been developed. This transformation is highly efficient with dissociation of six hydrogens including two sp³ C H and one sp² C H bond activations. This method not only provides an efficient approach to 2‐oxo‐acetamidine compounds, but also offers a valuable mechanistic insight into this novel copper catalysis.