The deprotonation of (µ -H)Fe3(CO)9(µ - CO)(µ3-HBH) with n-butyllithium yields the dianionic complex [Li]2[Fe3(CO)9(µ3 - HBCO)], which has been spectroscopically characterized. In contrast to the facile reprotonation of closely related ferraboranes, prctonation of [Li]2[Fe3(CO)9(µ 3- HBCO)] leads to decomposition. On the other hand, reaction of this dianionic complex with 2 equiv of FeCI3 gives a good yield of [LI] (Fe3(CO)9(µ -CO)( µ3-HBCI). Metathesis with [AsPh4][C1] yields [AsPh4] [Fe3(CO)9(µ -CO) (µ3-HBC1)], which has been crystallographically characterized (triclinic, Pī, a = 9.534(3) A, b = 13.305(4) A,, c = 15.225(4) A, α = 104.39(2)°, β = 103.56(2)°, Y = 99.23(2)0, V = 1768.7(8) A3, Z= 2). Comparison with the analogous osmium clusters, as well as isoelectronic organometallic clusters. reveals relationships among their structures, properties, and energetics.