Halogenotriphenyltin(IV) adducts of tetrakis(t-butyl isocyanide)-rhodium(I) perchlorate. Preparation and kinetics.
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概要
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[Rh(<I>t</I>-BuNC)<SUB>4</SUB>]ClO<SUB>4</SUB> undergoes oxidative addition reactions with Ph<SUB>3</SUB>SnX (X=Cl, Br) to give <I>cis</I>-[Rh-(Ph<SUB>3</SUB>Sn)X(<I>t</I>-BuNC)<SUB>4</SUB>]ClO<SUB>4</SUB>. The adducts partly dissociate in solution to exist as an equilibrium mixture with the Rh(I) substrate and the addendum. Kinetics of the equilibrium reactions in three different organic solvents were studied spectrophotometrically under pseudo-first-order conditions with excess Ph<SUB>3</SUB>SnX. Rate constants for the forward reaction (<I>k</I><SUB>f</SUB>) are strongly dependent on the solvent polarity; <I>k</I><SUB>f</SUB> increases in the order of 1,2-dichloroethane<acetone<acetonitrile, whereas those for the backward reaction are little dependent on the solvents. Activation parameters also were obtained for the X=Cl system in acetonitrile; Δ<I>S</I><SUP>\neweq</SUP> for the forward reaction is −99.2 J mol<SUP>−1</SUP> K<SUP>−1</SUP>, while that for the backward reaction is +24.9 J mol<SUP>−1</SUP> K<SUP>−1</SUP>. These results indicate that the addition reactions proceed <I>via</I> a three-center transition state formed by the nucleophilic attack of the Rh(I) ion to the tin atom.
- 公益社団法人 日本化学会の論文
著者
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Tanaka Toshio
Department of Applied Chemistry, Faculty of Engineering, Osaka Univeristy
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Kuwae Ryosho
Department of Applied Chemistry, Faculty of Engineering, Osaka University
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