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The reaction of the cycloheptatrienyl-toluene sandwich complex [(η 7 -C 7 H 7 )Mo(η 6 - C 6 H 5 Me)]BF 4  with tricyclohexylphosphine in acetonitrile furnishes the cationic half-sandwich cycloheptatrienyl complex {(η 7 -C 7 H 7 )Mo[P(C 6 H 11 ) 3 ](CH 3 CN) 2 }BF 4  (1). Treatment of 1 with NaBH 4  in ethanol results in the formation of the tetrahydroborate complex {(η 7 -C 7 H 7 )Mo(η 2 - BH 4 )[P(cyclo-C 6 H 11 ) 3 ]} (2), in which the borohydride ligand is coordinated to the molybdenum atom through two three-center, two-electron bonds. The complex is stable in ethanol and water. The expected formation of a metal trihydride of the type {(η 7 -C 7 H 7 )MoH 3 [P(cyclo-C 6 H 11 ) 3 ]} as a hydrolysis product could not be observed. Since this behaviour differs from the reactivity reported for related cyclopentadienyl-ruthenium complexes, a comparative computational study on the model complexes [(η 5 -C 5 Me 5 )RuH 3 (PMe 3 )] (4) and [(η 7 -C 7 H 7 )MoH 3 (PMe 3 )] (5) was performed revealing that the classical trihydride form [MH 3 ] represents the global minimum for the ruthenium complex 4, whereas the dihydrogen-hydride form [MH(η 2 -H 2 )] is more stable for the molybdenum counterpart.

zeitschrift für naturforschung b

Synthesis, Structure and Reactivity of the Molybdenum Cycloheptatrienyl Tetrahydroborate Complex {(η 7 -C 7 H 7 )Mo(η 2 -BH 4 )[P(cyclo-C 6 H 11 ) 3 ]}