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• W2065504816 abstract "Relative bond dissociation energies (BDEs) have been obtained by equilibrating early transition metal alkyls and hydrides with H2 or the CH bonds of hydrocarbons. Thus, in benzene solution Cp2HfH2 (CP = (η5-C5Me5)) equilibrates with Cp2Hf(C6H5)H and dihydrogen. From the enthalpy of the reaction, ΔHO = +6.0(3), the HfH (BDE) is calculated to be 0.8(3) kcal mol−1 stronger than the HfC6H5BDE. Relative ScC6H5 and Scalkyl BDEs have been estimated from the equilibration of the metallated complex Cp(η5,η1-C5Me4CH2CH2CH2)Sc, C6H6 and Cp(η5-C5Me4CH2CH2CH3)ScC6H5, the ScC6H5 BDE being 16.6(3) kcal mol−1 stronger than the ScCH2CH2CH2C5Me4 BDE. From a similar reversible intramolecular metallation of Cp(η5-C5Me4CH2CH2CH3)HfH2 to give Cp(η5,η1-C5Me4CH2CH2CH2)HfH and dihydrogen, the HfH BDE is estimated to be 23.0(3) kcal mol−1 stronger than the HfCH2CH2CH2C5Me4 BDE. The equilibration of Cp(η5-C5Me4CH2C6H5)ScCCCMe3 with metallated scandocene derivative Cp(η5,η1-C5Me4CH2-o-C6H4)Sc and tert-butylacetylene lies very far towards Cp(η5- C5Me4CH2C6H5)ScCCCMe3, so that only a lower limit for the relative Scalkynyl and Scaryl BDEs may be determined: BDE(Scalkynyl)-BDE(Scaryl) >29(5) kcal mol−1. These early transition metal-hydrocarbyl (MR) BDEs correlate with the corresponding HR BDEs (i.e. Malkynyl > Maryl > Malkyl); however, the MR BDEs increase more rapidly with s character for R than do the HR BDEs. The origin of this effect is not known, but it is undoubtedly also responsible for the characteristically high MH BDEs for transition metal hydride compounds. In order to probe the polarity of Scaryl bonds a series of scandocene derivatives capable of reversibly metallating at either of two differently substituted benzyl groups was prepared. The equilibrium constants for these metallated derivatives: (η5,η1-C5Me4CH2-o-C6H3-p-X)(η5-C5Me4CH2C6H4-m- CH3)Sc (η5-C5Me4CH2C6H4-m-X)(η5,η1-C5Me4CH2-o-C6H3-p-CH3)Sc (X = H, CF3, NMe2) were determined. The small dependence of Keq on the nature of X suggests that the Scaryl bond is essentially covalent with only a small ionic contribution." @default.
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• W2065504816 title "Relative bond dissociation energies for early transition metal alkyl, aryl, alkynyl and hydride compounds. Equilibration of metallated cyclopentadienyl derivatives of peralkylated hafnocene and scandocene with hydrocarbons and dihydrogen" @default.
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• W2065504816 doi "https://doi.org/10.1016/s0277-5387(00)81771-4" @default.
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