Cyclic voltammetry of Rh(I) complexes and the oligomers. A correlation between the anodic peak potentials and the rate constants for the electron transfer reactions with inorganic oxidants.
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概要
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The cyclic voltammogram of a CH<SUB>3</SUB>CN solution of [Rh(<I>p</I>-MeOC<SUB>6</SUB>H<SUB>4</SUB>NC)<SUB>4</SUB>]<SUP>+</SUP> exhibits three anodic current peaks which correspond to the oxidations of the monomer, the dimer, and the trimer, with no cathodic wave on the reverse scan. The anodic peak potentials <I>E</I><SUB>ox</SUB><SUP>p</SUP> in such irreversible cyclic voltammograms were determined for various Rh(I) monomers and the oligomers such as [Rh(RNC)<SUB>4</SUB>]<SUP>+</SUP>, [Rh<SUB>2</SUB>(RNC)<SUB>8</SUB>]<SUP>2+</SUP>, [Rh<SUB>2</SUB>(dppm)<SUB>2</SUB>(RNC)<SUB>4</SUB>]<SUP>2+</SUP>, [Rh<SUB>2</SUB>(dicp)<SUB>4</SUB>]<SUP>2+</SUP>, [Rh<SUB>3</SUB>(RNC)<SUB>12</SUB>]<SUP>3+</SUP>, and [Rh<SUB>4</SUB>(dicp)<SUB>8</SUB>]<SUP>4+</SUP> (R=<I>p</I>-MeOC<SUB>6</SUB>H<SUB>4</SUB> and Ph, <I>etc</I>; dppm=bis(diphenylphosphino)methane, dicp=1,3-diisocyanopropane). The anodic peak potentials <I>E</I><SUB>ox</SUB><SUP>p</SUP> vary mainly with the degree of oligomerization of the Rh(I) complexes, decreasing in the order monomer>dimer>trimer>tetramer, in parallel with the energies of the highest occupied molecular orbitals <I>E</I><SUB>HOMO</SUB>. It has been found that the <I>E</I><SUB>ox</SUB><SUP>p</SUP> values are linearly correlated with logarithm of the rate constants for the electron transfer reactions with inorganic oxidants such as [Fe(bpy)<SUB>3</SUB>]<SUP>3+</SUP> and [Co(bpy)<SUB>3</SUB>]<SUP>3+</SUP> (bpy=2,2′-bipyridine) in the context of the Marcus theory as expected when the standard oxidation potentials <I>E</I><SUB>ox</SUB><SUP>o</SUP> would be used. It is thus suggested that the anodic peak potentials of the Rh(I) complexes in the irreversible system can be used as the standard oxidation potentials as far as the relative values are concerned.
- 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
-
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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