合成气聚合转化烷烯烃基础研究
发布时间：2018-07-17 18:45
【摘要】：本文针对合成气制备低碳烯烃中催化剂的制备关键技术问题,以堇青石为载体,铁基催化剂为主体,通过分析不同金属钼、镍的添加对催化剂性能的影响,研究了不同催化剂的物相、形貌、电子结合能等特征,以及制备催化剂过程中不同物质之间的质量比、载体堇青石的铝溶胶改性、助剂的添加量对催化剂性能的影响等。通过对反应因素,温度、合成气比例、空速进行探讨以获得最佳的催化活性。结果表明:(1)以堇青石为载体,铁和钼为主要原料制备的催化剂,具有分散活性组分的作用。SEM、EDX、FTIR、以及XPS等分析发现起活性作用的铁和钼分别以四氧化三铁和氧化钼的形式存在。该催化剂最佳的活性条件为:反应温度为450℃C、合成气比例为2、空速为2.0L/g cat-h,乙烯的选择性和原料气一氧化碳的转化率达到最大为53.8%和63.5%。(2)通过添加钾助剂对催化剂的电子结构以及通过铝溶胶对堇青石进行改进后,同样具有较好的催化效果。SEM、TEM、EDX、XRD、XPS等分析表明铝溶胶的改性增大催化剂的表面积,有利于活性组分的分散。钾助剂的添加更有利于铁物质以低价活性态形式存在。(3)当铁和钼的合成比例为1:1,钾助剂的含量为0.12wt%,铝溶胶改性堇青石等催化效果更佳。当反应温度为450℃C,合成气比例为1,空速为1200 mL/g cat-h的情况,一氧化碳的转化率最高为51.4%,乙烯的选择性也最大为25.2%。(4)铁基催化剂和镍基催化剂构成的双金属催化因堇青石的活性分散作用,对C2烃的选择性以及一氧化碳的转化率具有高效的活性。当反应温度为450℃C,合成气比例为2,空速为2800mL/gcat-h,其中C2烃的选择性最大为37.7%,乙烯的选择性为26.6%,一氧化碳的转化率为58.5%。
[Abstract]:In view of the key technical problems in the preparation of catalysts for the preparation of low olefins from syngas, cordierite was used as the carrier and iron based catalysts as the main body. The effects of the addition of different metal molybdenum and nickel on the performance of the catalysts were analyzed. The phase, morphology, electronic binding energy of different catalysts, the mass ratio of different materials in the preparation of the catalyst, the modification of cordierite supported by aluminum sol, and the effect of additives on the performance of the catalyst were studied. The optimum catalytic activity was obtained by discussing the reaction factors, temperature, syngas ratio and space velocity. The results showed that: (1) the catalysts prepared with cordierite as the carrier and iron and molybdenum as the main raw materials had the effect of dispersing the active components. The results of FTIR and XPS analysis showed that the active iron and molybdenum existed in the form of Fe _ 2O _ 3 and Mo _ 2O _ 3, respectively. The optimum conditions are as follows: the reaction temperature is 450 鈩，
本文编号：2130591
[Abstract]:In view of the key technical problems in the preparation of catalysts for the preparation of low olefins from syngas, cordierite was used as the carrier and iron based catalysts as the main body. The effects of the addition of different metal molybdenum and nickel on the performance of the catalysts were analyzed. The phase, morphology, electronic binding energy of different catalysts, the mass ratio of different materials in the preparation of the catalyst, the modification of cordierite supported by aluminum sol, and the effect of additives on the performance of the catalyst were studied. The optimum catalytic activity was obtained by discussing the reaction factors, temperature, syngas ratio and space velocity. The results showed that: (1) the catalysts prepared with cordierite as the carrier and iron and molybdenum as the main raw materials had the effect of dispersing the active components. The results of FTIR and XPS analysis showed that the active iron and molybdenum existed in the form of Fe _ 2O _ 3 and Mo _ 2O _ 3, respectively. The optimum conditions are as follows: the reaction temperature is 450 鈩，
本文编号：2130591
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