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STUDY OF FISCHER-TROPSCH SYNTHESIS OVER A SILICA SUPPORTED IRON CATALYST THROUGH THE USE OF REACTIVE SCAVENGERS.

机译:通过使用反应性增溶剂在二氧化硅支撑的铁催化剂上合成费-托合成的研究。

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The synthesis of hydrocarbons from H(,2) and CO was studied on a silica-supported Fe catalyst. The synthesis was carried out at 1.54 atm and 200 to 255(DEGREES)C in a differential reactor. Conversion of CO never exceeded 2%. The working catalyst was achieved by transforming Fe(,2)O(,3) into a mixture of Fe(,3)O(,4), bulk carbides, and iron under synthesis conditions. Synthesis product distributions and the rate of methane formation are reported. Trends in CO(,2) formation and the presence of cyclic hydrocarbons, saturated and unsaturated, suggest the presence of some Fe(,3)O(,4) at the catalyst surface. Cyclohexene addition to the feed generated low concentrations of alkyl-substituted cyclohexene and cyclohexanes consistent with reported scavenging studies over Ru. Pyridine addition to the feed generated alkyl-substituted pyridines. Additional experiments confirmed that scavenged products are not formed from the interactions between the scavenger and synthesis products on support. The results confirm that the scavengers react with species involved in chain propagation.; Pyridine was used to scavenge C(,1)-C(,3) alkyl species from the catalyst surface. The (alpha)-alkylpyridine distributions were dependent upon synthesis variables and demonstrated a dependence which was proportional to the dependence of C(,1)-C(,3) Fischer-Tropsch products. These results confirmed that alkyl species are the immediate precursors to synthesis products. Two most probably Fischer-Tropsch mechanisms were used to describe the catalytic behavior and scavenged product distributions. The alkyl fragment dependences were predicted using Langmuir-Hinshelwood expressions for these two mechanisms and were compared against the measured scavenged dependence. Lack of information concerning CO adsorption characteristics at synthesis conditions prevented discrimination between the possible mechanisms.
机译:在二氧化硅负载的Fe催化剂上研究了由H(,2)和CO合成碳氢化合物。在差分反应器中于1.54atm和200至255(DEGREES)C下进行合成。一氧化碳的转化率从未超过2%。通过在合成条件下将Fe(,2)O(,3)转变为Fe(,3)O(,4),块状碳化物和铁的混合物来获得工作催化剂。报告了合成产物分布和甲烷形成速率。 CO(,2)形成的趋势以及饱和和不饱和环状烃的存在表明催化剂表面存在一些Fe(,3)O(,4)。进料中环己烯的添加产生了低浓度的烷基取代的环己烯和环己烷,这与报道的对Ru的清除研究一致。将吡啶添加到进料中产生烷基取代的吡啶。另外的实验证实清除剂不是由载体上的清除剂与合成产物之间的相互作用形成的。结果证实了清除剂与参与链传播的物种反应。吡啶用于从催化剂表面清除C(,1)-C(,3)烷基物质。 α-烷基吡啶的分布取决于合成变量,并显示出与C(,1)-C(,3)费-托产物的依赖性成比例的依赖性。这些结果证实了烷基物质是合成产物的直接前体。两种最可能的费-托机理用于描述催化行为和清除的产物分布。使用Langmuir-Hinshelwood表达式对这两种机理预测了烷基片段的依赖性,并将其与测得的清除依赖性进行了比较。缺乏有关合成条件下CO吸附特性的信息,无法区分可能的机理。

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