An Electron-Deficient Iridium(III) Dihydride Complex Capable of Intramolecular CH Activation

Double take: A remarkable electron‐deficient cationic dihydride complex [Ir(ItBu)2(H)2](PF6) (see crystal structure), prepared in high yield from the reaction of 14‐electron complex [Ir(ItBu′)2](PF6) and H2 gas, shows a rare agostic interaction. The reaction illustrates the reversibility of a double, intramolecular CH activation process and provides a rare example of a “proposed” intermediate. ItBu: N,N′‐di(tert‐butyl)imidazol‐2‐ylidene.