Electron transfer activation in the oxidative addition of iodine to rhodium(I) complexes.
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概要
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The kinetics of the oxidative addition of iodine to the following isocyaniderhodium(I) monomers and dimers in MeCN has been examined; [Rh(RNC)<SUB>4</SUB>]<SUP>+</SUP>, [Rh(RNC)<SUB>2</SUB>(PPh<SUB>3</SUB>)<SUB>2</SUB>]<SUP>+</SUP>, [Rh<SUB>2</SUB>(dppm)<SUB>2</SUB>(RNC)<SUB>4</SUB>]<SUP>2+</SUP>, and [Rh<SUB>2</SUB>(dicp)<SUB>4</SUB>]<SUP>2+</SUP> (R=alkyl, aryl; dppm=bis(diphenylphosphino)methane; dicp=1,3-diisocyanopropane). The reaction proceeds <I>via</I> two consecutive steps which consist of the formation of the initial adduct followed by the intramolecular isomerization to yield the final <I>trans</I>-adduct. The kinetic results for the first step of the oxidative addition reactions suggest that there exist three kinds of intermediates formed between the Rh(I) complex and iodine with 1:1, 1:2, and 2:1 stoichiometry prior to the formation of the initial adduct. This mechanism coincides with that for the electron transfer reactions between the Rh(I) complexes and inorganic oxidants such as [Fe(N-N)<SUB>3</SUB>]<SUP>3+</SUP> (N-N=1,10-phenanthroline and 2,2′-bipyridine). The values of the rate constants for the first step of the oxidative addition of iodine to dppm- or dicp-bridged Rh(I) dimers are found to agree with those for the electron transfer reactions between the same reactants by using linear free energy relationships. The possibility of electron transfer activation as the rate determining step in the oxidative addition to Rh(I) complexes is discussed.
- 公益社団法人 日本化学会の論文
著者
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Fukuzumi Shunichi
Department Of Applied Chemistry Faculty Of Engineering Osaka University
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Tanaka Toshio
Department of Applied Chemistry, Faculty of Engineering, Osaka Univeristy
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Nishizawa Nobuaki
Department of Applied Chemistry, Faculty of Engineering, Osaka University
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