“…12 The formation of an actinide ketimide complex ( 5 ) seems to be the crucial step in the synthesis of the unique 5,6‐dicyano‐1‐methyl‐3‐( N ‐methylamino)isoindolyl ligand. Numerous examples of metal‐mediated nitrile coupling reactions with compounds such as amines,13a imines,13b ketones,13c alkynes,13d amidines,13e oximes,13f and other nitriles13g are known. However, to the best of our knowledge, the coupling of a nitrile with a ketimide functional group has not been observed with transition metals, once again highlighting the differences between transition metals and the actinides.…”