Racemization and Isotopic Exchange of Tris(acetylacetonato)silicon(IV) Perchlorate in Organic Solvents
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概要
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Racemization of trisacetylacetonatosilicon(IV) ions and their isotopic exchange reaction with acetylacetone-<SUP>14</SUP>C (Hacac) have been studied in tetrachloroethane (TCE) and acetonitrile (AN). No solvolysis takes place at least below 60°C, and the racemization rate <I>R</I> is expressed as follows: <I>R</I>=[complex] (<I>k</I><SUB>1</SUB>+<I>k</I><SUB>2</SUB>[acid]) (in TCE) and <I>R</I>=[complex] (<I>k</I><SUB>3</SUB>+<I>k</I><SUB>4</SUB>[base]) (in AN). The rate constants and activation parameters at 50°C are as follows: rate constants, 4.79×10<SUP>6</SUP> s<SUP>−1</SUP>, 1.35×10<SUP>−4</SUP> M<SUP>−1</SUP> s<SUP>−1</SUP>, 3.87×10<SUP>−5</SUP> s<SUP>−1</SUP> and 1.19×10<SUP>−1</SUP> M<SUP>−1</SUP> s<SUP>−1</SUP>, activation enthalpy (<I>ΔH</I><SUP>\neweq</SUP>/kcal mol<SUP>−1</SUP>) 31.6±0.1, 29.3±1.9, 25.7±0.2 and <I>ca.</I> 18, and activation entropy (<I>ΔS</I><SUP>\neweq</SUP>/cal mol<SUP>−1</SUP>K<SUP>−1</SUP>) 14.6, 14.2, 0.53, −5.75, respectively, for <I>k</I><SUB>1</SUB>, <I>k</I><SUB>2</SUB> (for trichloroacetic acid), <I>k</I><SUB>3</SUB> and <I>k</I><SUB>4</SUB> (for 2,6-lutidine). No isotopic exchange is observed within 6 hr at 60°C in the solvents. The racemization should proceed intra-molecularly and presumably <I>via</I> an intermediate of coordination 5 with one of the ligands as unidentate.
- 公益社団法人 日本化学会の論文
著者
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Inoue Tomoaki
Department Of Applied Molecular Chemistry College Of Industrial Technology Nihon University
-
Saito Kazuo
Department Chemistry Faculty Of Science Tohoku University
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Inoue Tomoaki
Department of Chemistry, Faculty of Science, Tohoku University
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