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CO2的固定化——Pd/Cu/ZnO Nanocatalyst(JACS, Top20 Articles)

已有 5196 次阅读 2007-10-18 08:13 |个人分类:科研点滴启发

Most-Accessed Articles: April-June, 2007

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  • Carbon Dioxide Fixation into Chemicals (Methyl Formate) at High Yields by Surface Coupling over a Pd/Cu/ZnO Nanocatalyst
    K. M. Kerry Yu, Connie M. Y. Yeung, and Shik Chi Tsang
    J. Am. Chem. Soc.; 2007; 129(20) pp 6360 - 6361; (Communication) DOI: 10.1021/ja0706302
    Access: Abstract / Supporting Info

    这篇文章的主要内容以及亮点:

     由于环保要求(CO2是最基本的温室气体),an instantaneous response for research studies in the chemistry of CO2 including its activation,utilization, and fixation is urgently needed.

    目前主要措施:

    • the physical storage of CO2 into depleted oil/gas/coal reservoirs
    • chemical fixation of CO2 has attracted additional attention as a possible way to manufacture useful chemicals in some specific locations.

    但是CO2活化存在一定的问题、难度:

    Most previous attempts were unable to attract industrial attention as they suffer from either the use of expensive but non-robust homogeneous catalysts or the use of peculiar reaction conditions (requires excess ligand(s) and solvents at extreme conditions).

    本文主要工作:

    • a one-step catalytic fixation of CO2 to methyl formate (MF) in liquid phase under mild industrial applicable conditions by using a new concept of coupling surface formate species formed from CO2 on solid catalyst with excess methanol in hydrogen to form the MF,
    •  and the quantity of the product is found to greatly exceed the surface coverage of the catalyst by >45-fold. As a result, we report, for the first time, that the optimum Pd/Cu/ZnO/alumina nanocatalyst prepared from simple co-precipitation is capable of activating gaseous CO2 to condensable MF at high yields (>20%) with excellent selectivity (>96%).

     结论:

  • To conclude, it is demonstrated that, with introduction of methanol to the Pd/Cu/ZnO nanocatalyst under H2/CO2, carbon dioxide can be activated and fixed as methyl formate with impressive TOF, yield, and selectivity. Thus, a new route for CO2 activation by heterogeneous means at ambient conditions is described. This preliminary study also offers directions to rationally design and optimize the required catalyst, reactor, and experimental conditions for this reaction.

     

  • Carbon Dioxide Fixation into Chemicals (Methyl Formate)

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