Activation of Small Inorganic Molecules by M.M. Taqui Khan


By M.M. Taqui Khan

Activation Of Small Inorganic Molecules

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The rate-determining step of the reaction [Eq. (55)] appears to be the formation of this intermediate by the displacement of the coordinated chloride by a hydride ion. Reaction of (AsPh 3 ) 3 RuCl 2 with hydrogen in benzene containing ethanol or triethylamine gave a hydrido complex of the composition (AsPh 3) 3RuClH which has been isolated and characterized. 46 1. ACTIVATION OF MOLECULAR HYDROGEN L3R11CIX + olefin , L 3RuClX(olefin) c r Ru ci- 2 2 + H2 Ru t.. 3 kcal/mole and - 5 6 eu (L = AsPh 3), respectively.

IrH(CO)(PPh 3) 3 + H 2 Ir(H) 3(CO)(PPh 3)3 (67) A six-coordinate iridium(I) complex with the olefin as a ligand was also proposed [Eq. (68)]. IrH(CO)(PPh 3) 3 + C 2 H 4 I r ( C 2H 4) H ( C O ) ( P P h 3) 3 (68) The mechanism of the addition of the hydride ion to the olefin in the monohydrido complex should be different from that of the dihydrido complex, IrX(CO)(PPh 3) 2(H) 2, as indicated by the observed difference in the rates of hydrogénation in systems containing these complexes. The corresponding pentacoordinate rhodium(I) complex, RhH(CO)(PPh 3) 3, does not form the hydrogen adduct, but catalyzes the hydrogénation of ethylene and acetylene [182].

The final step is thus the reverse of the "aging" reaction for 3 [Co(CN) 5 ] -. In the case of allylic compounds in general, including halides, acetates, alcohols, ester, and amines, cleavage of the substrate takes place by reaction 3 with [Co(CN) 5 ] " to yield the allylpentacyanocobaltate(III) complex [127], as indicated in Scheme II. The rearrangement of the σ-bonded complex to a πallyl complex has been substantiated by measurement of the PMR spectra of mixtures of these complexes in D 2 0 Kwiatek [127] tentatively assigned 2 structure 28 to Tr-allyltetracyanocobaltate(III), C 3 H 5 Co(CN) 4 ~.

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