活性炭负载[Rh(COD)Cl]2催化剂的制备及其催化性能
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国家自然科学基金项目(面上项目,重点项目,重大项目)


Preparation and Catalytic Properties of [Rh(COD)Cl]2 Catalysts Supported on Activated Carbon
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The National Natural Science Foundation of China (General Program, Key Program, Major Research Plan)

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    摘要:

    制备了负载型[Rh(COD)Cl]2催化剂,用XPS、N2吸-脱附、FTIR对其结构进行表征与分析,以β-蒎烯加氢反应为探针反应,研究了载体种类、氧化剂HNO3浓度、Rh负载量对负载型[Rh(COD)Cl]2催化剂性能的影响,在此基础上优化了β-蒎烯加氢工艺条件,并测定了活性炭载[Rh(COD)Cl]2催化剂(缩写为[Rh(COD)Cl]2/AC)的重复使用性。结果表明,活性炭为较佳载体,在HNO3浓度为35%,Rh负载量为5%时,[Rh(COD)Cl]2在活性炭上的负载效果较好,且[Rh(COD)Cl]2/AC催化剂在β-蒎烯加氢反应中表现出较佳的催化活性,β-蒎烯转化率达99.0%以上,顺式蒎烷选择性高于89.0%,顺式蒎烷收率达88.9%以上。催化剂重复使用4次后,β-蒎烯转化率仍可达89.64%,活性组分Rh的流失是造成催化剂失活的主要原因。

    Abstract:

    Supported [Rh(COD)Cl]2 catalysts were prepared. The resulting catalysts were characterized by means of XPS, N2 adsorption-desorption and FTIR analysis methods. The hydrogenation reaction of beta-pinene was used as probe reactions to investigate the catalytic performance. The effects of carrier type, oxidant燞NO3 concentration and Rh-loading on catalytic properties were optimized in details. On this basis, the hydrogenation conditions were investigated by orthogonal爀xperiment, and the catalytic use of [Rh(COD)Cl]2/AC was measured as well. The experimental results indicated that the catalytic activity of [Rh(COD)Cl]2 catalysts supported on activated carbon was greatly improved. The catalyst showed optimal catalytic activities with 99.0% conversion of beta-pinene, 89.0% selectivity of cis-pinane and 88.9% yield of cis-pinane when the optimal conditions for catalyst preparation were carrier type of activated carbon, HNO3 concentration of 35% and Rh-loading of 5%. The [Rh(COD)Cl]2/AC remained high activities with 89.64% conversion of beta-pinene after being used for four times. The cause of deactivation of [Rh(COD)Cl]2/AC was that active component Rh was easy to lose in the running process.

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王红琴,王亚明,蒋丽红.活性炭负载[Rh(COD)Cl]2催化剂的制备及其催化性能[J].精细化工,2018,35(2):

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  • 收稿日期:2017-03-01
  • 最后修改日期:2017-06-01
  • 录用日期:2017-07-20
  • 在线发布日期: 2018-02-06
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