Four-component assembly of polysubstituted pyrimidines <i>via</i> dual C(sp ³ )–H functionalization of primary aliphatic amines

An efficient iodine-promoted four-component reaction has been developed for the synthesis of diverse polysubstituted pyrimidines from simple and readily available starting materials under metal-free conditions. The multicomponent strategy innovatively utilizes primary aliphatic amines as C-C-N synthons, aromatic aldehydes as C1 synthons and ammonium iodide as an environmentally benign nitrogen source, achieving α-C(sp³)-H and β-C(sp³)-H bond functionalization of primary aliphatic amines in one pot. This method offers a valuable alternative for synthesizing structurally diverse pyrimidines.