Catalyst-Free Cross-Dehydrogenative Coupling Strategy Using Air as an Oxidant: Synthesis of α‑Aminophosphonates

α-Aminophosphonates are synthesized by employing unfunctionalized starting materials using cross-dehydrogenative coupling strategy. This method does not require any catalyst and proceeds in the presence of open air as the only oxidant. Mechanistic studies revealed that the reaction is nucleophile dependent and specific to dialkyl phosphite and N-aryl tetrahydroisoquinoline derivatives.