Reactions of [Cp* Fe] with the Lewis acid [Zn(C F ) ] in the presence of [(PhC(S)S) ], 9,10-phenanthrenedione or 4,5-pyrenedione yield the salt [Cp* Fe][(PhC(S)S)Zn(C F ) ] 1, [Cp* Fe][((C H O )Zn(C F ) )⋅] 4, and [Cp* Fe][((C H O )Zn(C F ) )⋅] 5, respectively. The latter two species represent the first examples of isolable zinc-containing radical anions. While [(PhC(S)S) ] binds weakly to [Zn(C F ) ], the diones afford the isolable adducts [(C H O )Zn(C F ) ] 2 and [(C H O )Zn(C F ) ] 3. Cyclic voltammetry and computational studies support the view that 4 and 5 are formed via single electron transfer (SET) to the donor-acceptor adducts, 2 and 3, respectively. Subsequent treatment of 4 and 5 with [NC H NMe ] affords [Zn(C F ) (NC H NMe ) ] with liberation of the dione, and regeneration of [Cp* Fe].
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