化工进展 ›› 2021, Vol. 40 ›› Issue (3): 1449-1455.DOI: 10.16085/j.issn.1000-6613.2020-0872

• 工业催化 • 上一篇    下一篇

有序介孔材料Al-FDU-12的合成及其加氢精制应用

曹正凯1,2(), 张霞2, 段爱军1()   

  1. 1.中国石油大学(北京)重质油国家重点实验室,北京 102249
    2.中国石化大连石油化工研究院,辽宁 大连 116045
  • 收稿日期:2020-05-20 出版日期:2021-03-05 发布日期:2021-03-17
  • 通讯作者: 段爱军
  • 作者简介:曹正凯(1991—),男,博士研究生,研究方向为化学工程与技术。E-mail:1628889067@qq.com
  • 基金资助:
    国家自然科学基金(21878330)

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

CAO Zhengkai1,2(), ZHANG Xia2, DUAN Aijun1()   

  1. 1.State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China
    2.Dalian Research Institute of Petroleum and Petrochemicals, SINOPEC, Dalian 116045, Liaoning, China
  • Received:2020-05-20 Online:2021-03-05 Published:2021-03-17
  • Contact: DUAN Aijun

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X射线衍射(XRD)、广角XRD、N2吸附-脱附、扫描电镜(SEM)、透射电镜(TEM)和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、孔容以及比表面积大,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5.0MPa、质量空速(WHSV)1.0h-1、硅铝比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 catalysts NiMo/Al-FDU-12 were prepared by further impregnating nickel and molybdenum active metals. The Al-FDU-12 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 the NiMo/Al-FDU-12 with different Si and Al ratios were also evaluated. It showed that FDU-12 with high pore size, volume and surface area would lead to the 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 5.0MPa, WHSV of 1.0h-1, Si and Al atomic ratio of 20, the catalyst showed the highest hydrodesulfurization and denitrification activity. The desulfurization and denitrification rate could reach 98.9% and 95.3%, respectively. Under similar reaction conditions, the industrial catalyst presented lower hydrodesulfurization and denitrification activity than the 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, activity, petroleum, deactivation

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