Abstract: Al-FDU-12 mesoporous materials with different silicon-to-aluminum atomic ratios (Si/Al = 50, 40, 30, 20 and 10) were synthesized by in-situ synthesis, and the catalyst was prepared by further impregnating nickel and molybdenum active metals. The materials and catalysts were characterized by means of small-angle XRD, wide-angle XRD, N2 adsorption and desorption, SEM, TEM, UV and other characterization means. The hydrodesulfurization (HDS) performances of NiMo/Al-FDU-12 with different Si and Al ratios were also evaluated. It showed that FDU-12 material with high pore size, volume and surface area would allow high dispersion degree of active metals. The hydrodesulfurization and denitrification performances of NiMo/Al-FDU-12 catalyst were improved after Al modification. As the reaction conditions were: temperature of 350 ℃, hydrogen and oil volume ratio of 600, pressure of 5.0 MPa, WHSV of 1.0 h-1, Si and Al atomic ratio of 20, the catalyst has the highest hydrodesulfurization and denitrification activity. The desulfurization and denitrification rate could reach 98.9% and 95.3%, respectively. Under the similar reaction conditions, the industrial catalyst presented lower hydrodesulfurization and denitrification activity than NiMo/AF-20 and NiMo/AF-10 catalysts. Therefore, the FDU-12 materials after Al modification possessed good prospect of industrial application.

Key words: catalyst, synthesis, reactivity, petroleum, deactivation

摘要： 采用原位合成法合成了不同硅铝原子比（Si/Al=50、40、30、20、10）的Al-FDU-12介孔材料，进一步浸渍镍钼活性金属制备了催化剂。通过小角XRD、广角XRD、N2吸附脱附、SEM、TEM、紫外等表征手段对材料及催化剂做了相应的表征，并且考察了不同硅铝比的NiMo/Al-FDU-12催化剂在催化裂化柴油中的加氢脱硫脱氮性能。结果表明，FDU-12介孔材料孔径、孔容以及表面积大，活性金属分散度高。铝改性后的NiMo/Al-FDU-12催化剂加氢脱硫、脱氮活性得到显著提高。当反应条件为：温度350℃，氢油体积比600，压力5.0 MPa，WHSV 1.0 h-1时，硅铝比为20时，催化剂的加氢脱硫脱氮活性最高，脱硫率可达98.9%，脱氮率可达95.3%。在相同反应条件下，工业催化剂催化柴油加氢脱硫、脱氮率低于NiMo/AF-20以及NiMo/AF-10催化剂。因此，铝改性后的FDU-12材料具有良好的工业应用前景。

关键词: 催化剂, 合成, 活性, 石油, 失活