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    气相法制备1,1-二氯乙烯催化剂的稳定性研究

    Stability of the Catalyst for Gas Phase Synthesis of 1, 1-Dichloroethene

    • 摘要: 气相法制备1,1-二氯乙烯具有环境友好、原子利用率高等特点。考察了活性炭、二氧化硅和氧化铝气相催化1,1,2-三氯乙烷脱HCl合成1,1-二氯乙烯反应性能,通过BET(Brunauer-Emmett-Teller area)、EDS(Energy Dispersive Spectrometer)、TG-MS(Thermal Gravity Analysis-mass spectrometry)、XRD(X-ray diffraction)等表征以及对失活催化剂的原位高温处理,分析了活性炭的高稳定性和失活机理。结果显示:在温度300℃、常压、氮气30 mL·min-1、催化剂体积0.4 mL条件下,活性炭稳定性远高于二氧化硅和氧化铝;二氧化硅单位时间单位面积的积炭量最多为146.3×10-7 g,氧化铝居中为91.4×10-7 g,活性炭最少为1.1×10-7 g;失活催化剂在空气中经原位高温再生处理后活性恢复,而在氮气中未恢复,表明积炭是导致催化剂失活的主要因素。

       

      Abstract: Dehydrochlorination of 1,1,2-trichloroethane to prepare 1,1-dichloroethene using solid catalysts in gas phase is an environmental friendly process, and almost 100% effective atom utilization can be achieved. Catalytic performance of activated carbon, silica and alumina for 1,1,2-trichloroethane dehydrochlorination to prepare 1,1-dichloroethene was investigated. The high stability of activated carbon and deactivation mechanism were analyzed by BET, EDS, TG-MS, XRD, and comparison experiments between fresh and deactivated catalysts with high temperature treatment were studied. The results show that the stability of activated carbon is far better than silica and alumina when studied under 300℃, 1 atmosphere, 30 mL·min-1 N2 and 0.4 mL of catalyst. Silica has the maximum carbon deposition quantity per unit time per unit area of 146.3×10-7 g, while alumina and activated carbon have a medium value of 91.4×10-7 g and 1.1×10-7 g, respectively. The deactivated catalysts can regain activity after high temperature treatment in air but not in N2. The results suggest that catalyst deactivation is mainly caused by carbon deposition.

       

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