Chinese Journal of Catalysis ›› 2015, Vol. 36 ›› Issue (7): 1001-1008.DOI: 10.1016/S1872-2067(15)60855-5

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Incorporation of Al3+ ions to promote the stabilization effect of (NH4)2SiF6 treatment on the hydrothermal stability of mesoporous SBA-15 zeolite

Chenglong Zoua, Guanyu Shab, Yao Huangb, Guoxing Niua, Dongyuan Zhaoa   

  1. a Department of Chemistry, Fudan University, Shanghai 200433, China;
    b Department of Materials Science, Fudan University, Shanghai 200433, China
  • Received:2015-02-08 Revised:2015-03-25 Online:2015-06-12 Published:2015-07-30
  • Supported by:

    This work was financially supported by the National Basic Research Program of China (973 Program, 2010CB226901, 2013CB934100) and the National Natural Science Foundation of China (U1463206).

Abstract:

This work demonstrates an improved (NH4)2SiF6 treatment to enhance the hydrothermal stability of mesoporous SBA-15 zeolite. In this treatment, Al3+ ions are incorporated into SBA-15 zeolite first, then it is treated with 5% (NH4)2SiF6 solution according to 1% SiO2 of SBA-15 and finally washed with HCl (2 mol/L) to remove the pre-incorporated Al3+ ions. The obtained SBA-15 exhibits higher hydrothermal stability than that without pre-incorporated Al3+. Compared with the latter, the sample maintains a better ordered mesostructure and a larger surface area (271 m2/g) after hydrothermal treatment at 800 ℃ for 12 h in 100% steam. The results show that incorporating Al3+ ions into SBA-15 zeolite before (NH4)2SiF6 treatment obviously promotes the stabilization effect of (NH4)2SiF6 treatment. The mechanism suggests that the incorporated Al3+ ions can effectively capture F- ions that have been released from (NH4)2SiF6, and thus reduce their etching into the SBA-15 zeolite framework. This ensures that the positive factors of (NH4)2SiF6 treatment, such as silicon insertion and surface hydrophobization by F- ions, play effective roles in the improvement of the hydrothermal stability of SBA-15 zeolite. This promoting effect of the Al3+ ions is closely related to the method that is used to introduce the Al3+ and the SBA-15 zeolite processing temperature.

Key words: SBA-15 zeolite, Mesoporous material, Hydrothermal stability, Ammonium fluorosilicate, Al3+ ion incorporation, Si insertion