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在流化床反应条件下进行了SAPO-34催化的甲醇转化的程序升温反应,并分析了不同反应温度阶段的积碳产物.结合对反应流出物的检测结果和热分析及色质联用分析确定的积碳物种变化,解释了程序升温反应过程中甲醇转化特殊的变化趋势.在程序升温甲醇转化的积碳产物中,除芳烃外,还有一种饱和的多环烷烃积碳物种,它的生成影响了烃池活性中心的形成并引起甲醇转化在低温反应阶段的失活.甲基取代苯和甲基取代金刚烷是低温条件下SAPO-34催化的甲醇转化产生的主要积碳产物,它们在升温过程中会向甲基取代萘以及稠环芳烃转变.积碳物种的演变对应了甲醇转化在起始反应阶段(300~325oC)的反应活性升高和此后(325~350oC)的失活以及在更高温度阶段(350~400oC)活性的恢复.在反应性能评价和积碳分析基础上,首次提出了一种与金刚烷类积碳物种生成相关的低温甲醇转化的失活机理.
The temperature-programmed reactions of methanol conversion catalyzed by SAPO-34 were carried out under fluidized bed reaction conditions, and the products of carbon deposition at different reaction temperature stages were analyzed. Combined with the detection results of reaction effluents and thermal analysis and GC-MS To determine the change of carbon deposit species and explain the special trend of methanol conversion in the process of temperature rising reaction.At the same time, there is a kind of saturated polycyclic alkane carbon deposit in the process of methanol conversion, Formation affected the formation of active sites in the hydrocarbon pool and led to the deactivation of methanol conversion at low temperature.Methyl Substituted Benzene and Methyl-Substituted Adamantane are the major carbon products produced by the conversion of methanol catalyzed by SAPO-34 at low temperature, The conversion of methyl-substituted naphthalene to condensed-ring aromatics during the warming process is followed by the evolution of carbon species corresponding to the increased reactivity of methanol conversion during the initial reaction stage (300-325oC) and deactivation thereafter (325-350oC) And the recovery of activity at higher temperature (350 ~ 400oC) .According to the reactivity evaluation and carbon deposition analysis, a low temperature a Deactivation of transformation.