The thermal reactions of [MoH4(dppe)2] (1, dppe = Ph2PCH2CH2PPh2) with RSiH2X afford [MoH2X(dppe){[Ph2PCH2CH2P(Ph)C6H4-o]RXSi-P,P,Si}] (R = Ph, X = Cl (5a); R = cyclo-C6H11, X = Cl (5b); and R = Ph, X = Br (6)) by activation of the Si–H bond of the silanes and the ortho C–H bond of the phenyl group in the dppe ligand. Reduction of the Si–Cl and Mo–Cl bonds in 5a with LiAlH4 leads to the formation of the original complex 1 as a result of unusual Si–C bond cleavage. Meanwhile, dehalogenative reduction of 5a using zinc metal gives the known compound [MoH3{[Ph2PCH2CH2P(Ph)C6H4-o]2(Ph)Si-P,P,P,P,Si}] (2). The experimental results reported herein provide certain evidence for the involvement of the silylene species in the unusual formation of the present polydentate phosphinoalkyl–silyl ligands.
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