化工进展

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有序介孔材料Al-FDU-12的合成及其加氢精制应用

曹正凯1,张霞2,段爱军3   

  1. 1. 中国石油大学(北京)
    2. 中国石油化工股份有限公司大连石油化工研究院
    3. 中国石油大学(北京)重质油国家重点实验室
  • 收稿日期:2020-05-20 修回日期:2020-08-22 发布日期:2021-02-26
  • 通讯作者: 段爱军
  • 基金资助:
    国家自然科学基金

Synthesis of well ordered Al-FDU-12 mesoporous materials and their application on hydrogenation

  • Received:2020-05-20 Revised:2020-08-22 Published:2021-02-26

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

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

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