Multi-Talented Gallaphosphene for Ga-P-Ga Heteroallyl Cation Generation, CO2 Storage, and C(sp3 )-H Bond Activation.

Gallaphosphene L(Cl)GaPGaL (2; L=HC[C(Me)N(2,6-i-Pr2 C6 H3 )]2 ), which is synthesized by reaction of LGa(Cl)PCO (1) with LGa, reacts with [Na(OCP)(dioxane)2.5 ] to LGa(OCP)PGaL (3), whereas chloride abstraction with LiBArF 4 yields [LGaPGaL][BArF 4 ] (4; BArF 4 =B(C6 F5 )4 ). 4 represents a heteronuclear analog of the allyl cation according to quantum chemical calculations. Remarkably, 2 reversibly reacts with CO2 to yield L(Cl)Ga-P[μ-C(O)O]2 GaL (5), while reactions with acetophenone and acetone selectively give compounds 6 and 7 by C(sp3 )-H bond activation.