31P NMR study of active species for ethylene dimerization in .SIGMA.-aryl nickel complex-AgClO4.
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概要
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[NiBr(σ-C<SUB>6</SUB>F<SUB>5</SUB>)(PPh<SUB>3</SUB>)<SUB>2</SUB>] and [NiCl(σ-C<SUB>6</SUB>Cl<SUB>5</SUB>)(PPh<SUB>3</SUB>)<SUB>2</SUB>] are active for ethylene dimerization in the presence of AgClO<SUB>4</SUB>. The activity increases with increase in the amount of AgClO<SUB>4</SUB> and reaches maximum at AgClO<SUB>4</SUB>/Ni-complex=2. Addition of excess AgClO<SUB>4</SUB> leads to marked decrease in activity with [NiBr(σ-C<SUB>6</SUB>F<SUB>5</SUB>)(PPh<SUB>3</SUB>)<SUB>2</SUB>] but a little decrease with [NiCl(σ-C<SUB>6</SUB>Cl<SUB>5</SUB>)(PPh<SUB>3</SUB>)<SUB>2</SUB>]. <SUP>31</SUP>P NMR spectra of the active solution showed new resonance peaks due to [Ni(ClO<SUB>4</SUB>)(σ-C<SUB>6</SUB>X′<SUB>5</SUB>)(PPh<SUB>3</SUB>)<SUB>2</SUB>] and [Ni(ClO<SUB>4</SUB>)(σ-C<SUB>6</SUB>X′<SUB>5</SUB>)(PPh<SUB>3</SUB>)] (X′=F,Cl), accompanying formation of AgX (X=Br,Cl) and [Ag(ClO<SUB>4</SUB>)(PPh<SUB>3</SUB>)]. Thus the role of AgClO<SUB>4</SUB> is to abstract halide anion and/or triphenylphosphine. The amount of Ni(ClO<SUB>4</SUB>)(σ-C<SUB>6</SUB>X′<SUB>5</SUB>)(PPh<SUB>3</SUB>)] is in good correlation with the rate of dimerization, which suggests this species to be catalytically active.
- 公益社団法人 日本化学会の論文
著者
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Maruya Ken-ichi
Research Laboratory Of Resources Utilization Tokyo Institute Of Technology
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Nakamura Yoshiyuki
Research Laboratory Of Resources Utilization Tokyo Institute Of Technology
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Ishimura Yoshimasa
Research Institute for Radiation Biology and Medicine, Hiroshima University
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Ozaki Atsumu
Research Laboratories of Resources Utilization, Tokyo Institute of Technology
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Mizoroki Tsutomu
Research Laboratory of Resources Utilization, Tokyo Institute of Technology
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