常压制备纳米锰氧气凝胶载体氧化羰基化合成DPC
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摘要
分别采用柠檬酸络合常压干燥法、环氧丙烷促凝冷冻干燥法制备了三种纳米锰氧气凝胶材料。利用X射线衍射(XRD)、比表面积测定(BET)、扫描电镜(SEM)、高分辨电镜(HRTEM)等测试手段对不同方法制备的样品进行表征。结果表明:当加入TAA时,环氧丙烷促凝冷冻干燥法制备的纳米锰氧气凝胶材料呈现纳米花菜状的多晶结构,具有良好的量子效应。当负载质量分数为1%Pd后用于苯酚氧化羰基化合成碳酸二苯酯实验,当反应总压为5MPa(其中氧气体积分数约7%),反应温度70℃,反应时间4h时,碳酸二苯酯单程收率可达23.34%,选择性99.16%。该合成方法工艺简单,原料廉价易得,开辟了新的催化剂制备方法。
Three nano Mn oxide aerogels were prepared by the methods of citric acid complex via ambient drying, propylene oxide promoting freeze-drying, respectively. And the samples with different ways prepared were investigated by XRD, BET, SEM and HRTEM. The results show that nano Mn oxide aerogel using the propylene oxides promoting freeze-drying method present the nano cauliflower shape, which has a good quantum effects. After loading of mass fraction 1%Pd, which can be applied in the synthesis of diphenyl carbonate through oxidative carbonylation process, the single pass yield of catalyst obtained is 23.34% with the selectivity up to 99.16% when the total reaction pressure is 5 MPa(the volume fraction of oxygen is about 7%), reaction time is 6h and the reaction temperature is 70℃. As the process is simple and available, it offers a new approach to the catalyst preparation.
引文
[1]Cao A M,Hu J S,Liang H P,et al.Angewandte Chemie International Edition,2005,44(28):4391-4395.
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    [4]Viravaidya C,Li M,Mann S.Chemical communications,2004(19):2182-2183.

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