CoPc在八面沸石笼中的原位合成及性能研究

CoPc在八面沸石笼中的原位合成及性能研究

  • 摘要: 采用苯酐-尿素路线,对CoPc金属配合物在八面沸石超笼中原位合成进行了考察,并采用多种物化手段和催化反应对所制备的CoPcY进行了详细的表征。结果表明,该制备路线是一简便有效的合成路线,采用该路线可在八面沸石超笼中原位合成CoPc金属配合物并将之固定于八面沸石中。在该制备方法中合成温度、离子交换所采用的盐类型及催化剂对CoPc金属配合物在八面沸石超笼中的合成及所制备的CoPcY在环己烷氧化反应中的催化性能有很大的影响,其中180 ℃为最佳合成温度,氯化钴较适合作为交换的盐类。在八面沸石超笼中原位合成的CoPc金属配合物在温和的反应条件下对环己烷氧化具有良好催化活性,转化数TON最高可达5 000以上。

     

    Abstract: The phthalic anhydride-urea route was employed to in-situ synthesize CoPc in the supercages of zeolite Y. The prepared CoPcY was characterized by various physicochemical methods and catalytic reaction. The results show that the route is a simple and effective method for in-situ synthesis of CoPc complexes in the supercages of zeolite Y. In the route, the synthesis parameters (synthesis temperature, catalyst and salt used in ion exchange) have great influence on the properties of the prepared CoPcY, in which the optimum synthesis temperature for CoPc is 180℃ and a suitable salt for ion exchange is cobalt chloride. The CoPc in-situ synthesized in supercages of Zeolite Y by this route shows high catalytic activity for cyclohexane oxidation under mild reaction conditions, and TON is over 5 000 as H2O2 is used as oxidant, reaction temperature is 60 ℃ and reaction time is 10 h.

     

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