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Metallaboranes from Metal Carbonyl Compounds and Their Utilization as Catalysts for Alkyne Cyclotrimerization.

The photolysis of [M2 (CO)10 ] (M=Re or Mn) with BH3 ⋅thf at room temperature yields arachno-1 and 2, [(CO)8 M2 B2 H6 ] (1: M=Re, 2: M=Mn). Both the compounds show a butterfly structure with seven skeletal electron pairs and 42 valence electrons. This result presents a new method for general access to low-boron-content metal-boron compounds without the cyclopentadienyl ligand at the metal centers. This new synthetic route is superior to the existing procedures because it avoids the use of [LiBH4 ] and metal polychlorides, for which the synthesis is very tedious. Compound 1 catalyzes the cyclotrimerization of a series of internal and terminal alkynes to yield mixtures of 1,3,5- and 1,2,4-substituted benzenes. The reactivity of 1 with alkynes demonstrates for the first time that the introduction of the [B2 H6 ] moiety into the [Re2 (CO)10 ] framework significantly enhances the catalytic activity. Note that [Re2 (CO)10 ] catalyzes the same set of alkynes under harsh conditions over a prolonged period of time. Quantum-chemical calculations using DFT methods are applied to afford further insight into the electronic structure, stability, and bonding of 1 and 2. All the compounds are characterized by IR and 1 H, 11 B, and 13 C NMR spectroscopy, and the geometry of 1 is established unambiguously through crystallographic analysis.