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Dual-Bed Catalytic System for Direct Conversion of Methane to Liquid Hydrocarbons

机译:将甲烷直接转化为液态烃的双床催化系统

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摘要

A dual-bed catalytic system is proposed for the direct conversion of methane to liquid hydrocarbons. In this system, methane is converted in the first stage to oxidative coupling of methane (OCM) products by selective catalytic oxidation with oxygen over La-supported MgO catalyst. The second bed, comprising of the HZSM-5 zeolite catalyst, is used for the oligomerization of OCM light hydrocarbon products to liquid hydrocarbons. The effects of temperature (650-800℃), methane to oxygen ratio (4-10), and SiO_2/Al_2O_3 ratio of the HZSM-5 zeolite catalyst on the process are studied. At higher reaction temperatures, there is considerable dealumination of HZSM-5, and thus its catalytic performance is reduced. The acidity of HZSM-5 in the second bed is responsible for the oligomerization reaction that leads to the formation of liquid hydrocarbons. The activities of the oligomerization sites were unequivocally affected by the SiO_2/Al_2O_3 ratio. The relation between the acidity and the activity of HZSM-5 is studied by means of TPD-NH_3 techniques. The rise in oxygen concentration is not beneficial for the C_(5+) selectivity, where the combustion reaction of intermediate hydrocarbon products that leads to the formation of carbon oxide (CO+CO_2) products is more dominant than the oligomerization reaction. The dual-bed catalytic system is highly potential for directly converting methane to liquid fuels.
机译:提出了一种双床催化系统,用于将甲烷直接转化为液态烃。在该系统中,通过在La负载的MgO催化剂上用氧气进行选择性催化氧化,甲烷在第一阶段转化为甲烷(OCM)产物的氧化偶联。第二床由HZSM-5沸石催化剂组成,用于OCM轻烃产物低聚为液态烃。研究了温度(650-800℃),甲烷氧比(4-10),HZSM-5沸石催化剂的SiO_2 / Al_2O_3比对工艺的影响。在较高的反应温度下,HZSM-5大量脱铝,因此其催化性能降低。第二床中HZSM-5的酸度负责低聚反应,导致形成液态烃。 SiO_2 / Al_2O_3的比值明确影响了低聚位点的活性。通过TPD-NH_3技术研究了酸度与HZSM-5活性之间的关系。氧浓度的升高不利于C_(5+)的选择性,其中导致形成碳氧化物(CO + CO_2)的中间烃产物的燃烧反应比低聚反应更占优势。双床催化系统具有将甲烷直接转化为液体燃料的巨大潜力。

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