Kinetic isotope effects in the H+C3H6.RAR.C3H7 reaction.
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概要
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The absolute rate constants of the addition of H and D atoms to propylene-<I>d</I><SUB>0</SUB> and -<I>d</I><SUB>6</SUB> have been measured by means of the pulse radiolysis-resonance absorption technique over the temperature range of 200–500 K. The rate constants obtained were well expressed by these Arrhenius equations: <I>k</I>(H+C<SUB>3</SUB>H<SUB>6</SUB>)=(3.00±0.38)exp[－(1612±66)⁄<I>RT</I>], <I>k</I>(H+C<SUB>3</SUB>D<SUB>6</SUB>)=(2.55±0.57)exp[－(1509±128)⁄<I>RT</I>], <I>k</I>(D+C<SUB>3</SUB>H<SUB>6</SUB>)=(1.99±0.05)exp[－(1550±15)⁄<I>RT</I>], and <I>k</I>(D+C<SUB>3</SUB>D<SUB>6</SUB>)=(2.20±0.27)exp[－(1587±67)⁄<I>RT</I>] in units of 10<SUP>－11</SUP> cm<SUP>3</SUP> molecule<SUP>－1</SUP> s<SUP>－1</SUP>. The unit of activation energy is cal mol<SUP>－1</SUP>. Practically no isotope effects attributable to the difference between C<SUB>3</SUB>H<SUB>6</SUB> and C<SUB>3</SUB>D<SUB>6</SUB> could be observed. This is similar to the kinetic isotope effects previously observed in the rate constants of the addition of H and D atoms to isotopic ethylenes. The theoretical rate constants of the above reactions have been calculated by the conventional activated complex theory using the potential energy surface drawn by the <I>ab initio</I> method; however, no agreement with regard to the isotope effects could be obtained between experiment and theory because of the difference between C<SUB>3</SUB>H<SUB>6</SUB> and C<SUB>3</SUB>D<SUB>6</SUB>. This also is similar to the isotope effects found in the H+C<SUB>2</SUB>H<SUB>4</SUB>→C<SUB>2</SUB>H<SUB>5</SUB> reaction.
著者
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Watanabe Toshifumi
Department of Applied Physics, Tokyo Institute of Technology
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Kyogoku Takeshi
Department of Applied Physics, Tokyo Institute of Technology
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Sato Shin
Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology
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Tsunashima Shigeru
Department of Applied Physics, Tokyo Institute of Technology
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Nagase Shigeru
Chemistry Division, Faculty of Education, Yokohama National University
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