负载β-Mo2N0.78催化剂上加氢脱硫和加氢脱氮反应行为的研究

负载β-Mo2N0.78催化剂上加氢脱硫和加氢脱氮反应行为的研究

  • 摘要: 在N2-H2下,利用程序升温还原氮化反应制备氧化铝负载的β-Mo2N0.78催化剂,并以苯并噻吩(BT)、二苯并噻吩(DBT)和喹啉为模型化合物,考察该催化剂的加氢脱硫、加氢脱氮活性和选择性。实验结果表明,升高反应温度和压力均提高催化剂的加氢脱硫、加氢脱氮活性;升高温度可同时改善DBT的直接脱硫和氢化脱硫,对选择性没有明显的影响;提高反应压力有利于加氢产物的生成;同时可以使联苯加氢转化为环己基苯。添加喹啉的加氢脱硫反应结果表明,含氮化合物的添加降低了催化剂加氢脱硫反应活性,抑制了氢化脱硫反应的发生。少量硫化合物的添加,使喹啉的转化率提高,还提高了脱氮率。

     

    Abstract: An alumina supported β-Mo2N0.78 catalyst was synthesized via temperature-programmed nitriding reaction in N2-H2 mixture gases. The catalytic activity and selectivity for hydrodesulfurization(HDS) and hydrodenitrogenation(HDN) were studied by using benzothiophene(BT), dibenzothiophene(DBT) and quinoline as model compounds. The experimental results show that the HDS and HDN activity increases with the increasing of reaction temperature and pressure. There is little effect of increasing temperature on HDS selectivity of DBT because of its simultaneous improvement of two parallel desulfurization reactions, direct desulfurization and hydrogenation followed by desulfurization. On the other hand, high pressure favors the progress of the latter reaction. The HDS results of BT and DBT with the addition of quinoline indicate that the addition of N-containing molecule decreases the HDS activity of catalyst and restrains the reaction of hydrogenation followed by desulfurization. With the addition of S-containing molecule, not only the conversion of quinoline improves, but also the HDN activity obviously increases.

     

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