Syntheses and structures of a stable gallole free of Lewis base coordination and its dianion

A stable Lewis base‐free gallole bearing a bulky Mes* group (=2,4,6‐(t‐Bu)3C6H2) was synthesized by the treatment of Mes*GaCl2 with a 3,6‐dilithio‐3,5‐octadiene derivative. Reduction of the gallole with lithium metal afforded the corresponding gallole dianion species as a lithium salt. Structures of the gallole and the lithium salt of the gallole dianion have been elucidated by using X‐ray crystallographic analysis, NMR spectroscopies, and density functional theory calculations.