Abstract
We present the isolation and reactivity of terminal gold(I) imido complexes, and report on the effect of capping alkali-cations. These anionic and strongly basic “super”-imide complexes engage in CH-bond auration including benzene and pyridine. They also mediate the dehydrogenation of dihydroanthracene and cyclohexadiene under the generation of dihydrogen or the elimination of sodium hydride. Mechanistic investigations (kinetics, isotope effects) and quantum chemical calculations reveal that the coordinating alkali-cations control the complexes’ reactivity with strong CH bonds.