A Serendipitous One‐Pot Cyanation/Hydrolysis/Enamide Formation: Direct Access to 3‐Methyleneisoindolin‐1‐ones

Abstract A direct, one‐pot conversion of 2’‐haloacetophenones to 3‐methyleneisoindolin‐1‐one scaffolds using CuCN as the sole reagent without the need for moisture‐free or anaerobic conditions is reported. This serendipitously discovered transformation with a broad substrate scope provides a significantly different route towards these important scaffolds. The scope of the method has also been further extended towards the synthesis of three special scaffolds, which are analogous to various bio‐active drugs.