The mixed-metal cubane-type clusters [(Cp*Mo)
3(
3-S)
4RuH
2(PR
3)][PF
6] [Cp* =
5-C
5Me
5; R = Ph (
2), Cy (
5)] were effective for theN-N bond cleavage of hydrazine and phenylhydrazine via adisproportionation reaction. The ammonia cluster [(Cp*Mo)
3(
3-S)
4Ru(NH
3)(PPh
3)][PF
6] (
3) and/or the unprecedented double-cubane-type cluster with bridging nitrogenous ligands [{(Cp*Mo)
3(
3-S)
4Ru}
2(
2-NH
2)(
2-NHNH
2)][PF
6]
2 (
4) were isolated from thereaction mixtures, and their structures were determined by X-raydiffraction studies.