论文部分内容阅读
利用转篮式无梯度反应器,在工业FeMn催化剂上,在较宽的工业操作相关的反应条件下进行了FT合成反应动力学研究.首次提出了利用转篮式无梯度反应器反应气氛和反应温度均一的优势,将烃生成反应动力学的估算从传统的对烃生成和水煤气变换这两类发生在不同活性中心的反应同时进行估算的方法中分离出来,简化了烃生成动力学模型的计算.在基于亚甲基插入的亚烷基机理动力学模型基础上,考虑到乙烯与催化剂表面强的相互作用,将乙烯和乙烷的生成动力学参数单独计算.动力学模型计算的链增长、烷烃和烯烃生成的活化能均与文献报道值具有较好的一致性.由FT合成动力学模型计算的合成气消耗速率、甲烷生成速率和C5+的生成速率较好地与实验值吻合.通过动力学模型并结合实验结果分析发现,未考虑除化学反应之外的非本征因素的烯烃再吸附动力学模型不能够正确预测烃产物分布偏离ASF规律及烯烷比随碳数增加而下降的现象.
The kinetics of FT synthesis was studied on a commercial FeMn catalyst under a wide range of industrial operation-related reaction conditions using a basket-type gradientless reactor. The reaction kinetics of the reaction in a basket-type gradientless reactor was first proposed Temperature homogeneity, the estimation of hydrocarbon formation kinetics is separated from the traditional method of simultaneous hydrocarbon and water gas shift reactions that occur at different active sites, simplifying the calculation of the hydrocarbon formation kinetic model Based on the kinetic model of alkylene mechanism based on methylene insertion, considering the strong interaction between ethylene and catalyst surface, the kinetic parameters of formation of ethylene and ethane were calculated separately.Chain growth calculated by kinetic model, The activation energies of alkanes and alkenes are in good agreement with those reported in the literature.The syngas consumption rate, methane production rate and the formation rate of C5 + calculated by the FT synthesis kinetics model are in good agreement with the experimental values, The model and experimental results show that the kinetic model of olefin reabsorption without extrinsic factors other than chemical reaction is not considered Possible to accurately predict the hydrocarbon product distribution law and alkenyl alkoxy departing ASF ratio decreases with increasing carbon number of phenomenon.