Substrate‐induced Selective α‐C(sp3)−H Activation of N‐alkyl Amines: Synthesis of Coumarin‐fused Quinolinones under Air

Abstract A substrate‐induced synthesis of coumarin‐fused quinolinones is achieved from 4‐(phenylamino)‐2 H ‐chromen‐2‐ones using N ‐alkyl amines as the solvent and a carbon source under air conditions without any catalysts in one pot. This protocol highlights the special roles of 4‐(phenylamino)‐2 H ‐chromen‐2‐ones which were not only used as reactants but also as an internal oxidant selectively activated N ‐ α ‐C( sp 3 )−H bond. This reaction features catalyst‐free, broad substrate scopes ( N ‐alkyl amines 27 examples and quinolinones 24 examples), operationally simple for the one‐step synthesis, and recovery and recycling of the solvent.