A facile and general synthesis of 2,4,6‐triaryl pyrimidines has been developed. It involves a one‐pot [2+1+1+1+1] pseudo five‐component annulation of one methyl ketone, two aldehydes and two NH4OAc catalyzed by TfOH. One C−C and four C−N bonds are formed during the oxidative annulation process. The reaction shows good tolerance of many important functional groups in air and produces only water as the coproduct, making this methodology a highly versatile alternative to the existing methods for structuring pyrimidine framework.

An efficient one-pot four-component condensation and cyclization of ketones with DMF and ammonium acetate for the synthesis of 2,4-diarylsubstituted pyridines promoted by Selectfluor has been achieved. Symmetrical pyridines were obtained selectively when non-methyl ketones were used as the starting materials. Two CÀ C and CÀ N bonds are formed during the oxidative cyclization process.[a] J.

An iodine-catalyzed double [4 + 2] oxidative annulation of ketones and diamines is described. A multi-pathway coupled domino strategy has been developed for the synthesis of substituted dimeric pyrazines under metal-free conditions. One CÀ C and four CÀ N bonds are formed during this double [4 + 2] oxidative annulation process from two ketones and two diamines.