甲烷无氧芳构化反应中钼基分子筛催化剂上积炭的表征

甲烷无氧芳构化反应中钼基分子筛催化剂上积炭的表征

  • 摘要: 利用化学方法对钼基分子筛催化剂上的CH2Cl2可溶性积炭和不可溶性积炭进行分离,并通过质谱、红外光谱、核磁共振等手段对积炭进行了表征。结果表明,可溶性积炭的主组分为一种非芳烃物质,它的组成不随反应时间、反应温度和催化剂的酸性的变化而变化。可溶性积炭分子对催化剂的活性影响不大。高不饱和度的稠环芳烃型不可溶性积炭分子是催化剂失活的主要原因。

     

    Abstract: To find out the essence of the coke deactivation and probe into the way of elimination of the coke deactivation over zeolite catalysts in methane non-oxidative aromatization, the coke soluble or insoluble in CH2Cl2 was separated. Its composition and property were characterized by MS and IR methods. It was found that the soluble coke mainly consists of non-aromatic hydrocarbons. Its composition did not change with the reaction time, reaction temperature and acidity of the catalyst. The souble coke which was the precursor of the insoluble coke did not affect the activity of the catalysts. The souble coke formed mainly in the pores of zeolite catalysts. The insoluble coke consisted of the condensed-aromatics type hydrocarbon. Its composition changed with the reaction time, reaction temperature and acidity of the catalyst. The insoluble coke was divided into two types: burning mainly at 798 K and 843 K respectively. The insoluble coke of the two types with different H/C might be the main reason for the deactivation of catalysts.

     

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