碳纳米管负载铑催化剂上丙烯氢甲酰化

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Effect of carbon nanotubes, as a novel support material, on the performance of Rh-catalyst supported by them was studied. Catalysts based on carbon nanotubes, SiO2, carbon nlolecular sieves, actiye carbon, and GDX-lo2(a copolymer of styrene with divinyIbenzene),were prepared, and their catalytic behaviors for propene hydroformylation were investigated and compared. The results showed that, over the carbon nanotubes-supported Rh-catalyst, C3H6 conversion and regioselectivity of butyric aldehyde (represented by n/i, a ratio of n-butyric aldehyde to its isomer, i-butyric aldehyde, in the products) were pronouncedly improved: the average turnover frequency(TOF) for the catalytic hydroformylation of propene was 0.079 s-1 at 393K, which was 2.1 times faster than that over the Wh catalyst based on SiO2, and the n/i ratio of the aldehyde products reached to 11.6, which was 1.9 times higher than that over the catalyst based on SiO2.The roles of six-membered C-ring at the surface of the carbon-nanotubes on the stability of the catalytically active Rh-complexes and of the tubular nanthchannel on the spatiospecific seletivity of reaction intermediate state and butyric aldehyde produced were discussed. Effect of carbon nanotubes, as a novel support material, on the performance of Rh-catalyst supported by them was studied. Catalysts based on carbon nanotubes, SiO2, carbon nlolecular sieves, actiye carbon, and GDX-lo2 (a copolymer of styrene with divinyIbenzene ), were prepared, and their catalytic behaviors for propene hydroformylation were investigated and compared. The results showed that, over the carbon nanotubes-supported Rh-catalyst, C3H6 conversion and regioselectivity of butyric aldehyde (represented by n / i, a ratio of n -butyric aldehyde to its isomer, i-butyric aldehyde, in the products) were pronounced improved: the average turnover frequency (TOF) for the catalytic hydroformylation of propene was 0.079 s-1 at 393K, which was 2.1 times faster than that over the Wh catalyst based on SiO2, and the n / i ratio of the aldehyde products reached to 11.6, which was 1.9 times higher than that over the catalyst based on SiO2. The roles of six-membered C-ring at the surface of the carbon- n anotubes on the stability of the catalytically active Rh-complexes and of the tubular nanthchannel on the spatiospecific seletivity of reaction intermediate state and butyric aldehyde produced were discussed.
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