Al3+离子介入提升(NH4)2SiF6对SBA-15介孔材料的水热稳定化作用

doi:10.1016/S1872-2067(15)60855-5

催化学报 ›› 2015, Vol. 36 ›› Issue (7): 1001-1008.DOI: 10.1016/S1872-2067(15)60855-5

Al³⁺离子介入提升(NH₄)₂SiF₆对SBA-15介孔材料的水热稳定化作用

邹成龙^a, 沙观宇^b, 黄曜^b, 牛国兴^a, 赵东元^a

a 复旦大学化学系, 上海200433;
b 复旦大学材料系, 上海200433

收稿日期:2015-02-08 修回日期:2015-03-25 出版日期:2015-06-12 发布日期:2015-07-30
通讯作者: 牛国兴电话: (021)51630205; 传真: (021)51630307; 电子信箱: gxniu@fudan.edu.cn
基金资助:
国家重点基础研究发展计划(973计划, 2010CB226901, 2013CB934100); 国家自然科学基金(U1463206).

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

Chenglong Zou^a, Guanyu Sha^b, Yao Huang^b, Guoxing Niu^a, Dongyuan Zhao^a

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).

摘要/Abstract

摘要：

提出了一种(NH₄)₂SiF₆处理提高SBA-15介孔材料水热稳定性的改良方法. 采用SBA-15介孔材料中预引入Al³⁺离子, 再进行1%SiO₂计量的(NH₄)₂SiF₆处理, 最后用强酸洗脱预引入的Al³⁺. 结果显示, 由此处理的SBA-15材料, 其水热稳定性明显优于相同条件下未预引入Al³⁺时(NH₄)₂SiF₆处理的样品. 两者在800 ℃、100%水蒸气处理12 h后, 虽然均能很好保持其介观有序度、形貌及六方孔道结构, 但前者的比表面积可高达271 m²/g, 而后者仅为224 m²/g. 表明Al³⁺离子介入能大幅度提升(NH₄)₂SiF₆处理对SBA-15介孔材料的稳定化作用. 这主要得益于预引入的骨架Al³⁺在保障(NH₄)₂SiF₆处理修复SBA-15材料表面缺陷和进行表面疏水化、提升其水热稳定性的同时, 能减缓(NH₄)₂SiF₆释放的多余F^-离子对SBA-15材料骨架的刻蚀破坏作用. Al³⁺离子介入的这种提升作用与其引入方式和SBA-15材料所经受的温度密切相关.

关键词: SBA-15沸石介孔材料, 水热稳定性, 氟硅酸铵, Al³⁺离子引入, 补硅

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

邹成龙, 沙观宇, 黄曜, 牛国兴, 赵东元. Al³⁺离子介入提升(NH₄)₂SiF₆对SBA-15介孔材料的水热稳定化作用[J]. 催化学报, 2015, 36(7): 1001-1008.

Chenglong Zou, Guanyu Sha, Yao Huang, Guoxing Niu, Dongyuan Zhao . Incorporation of Al³⁺ ions to promote the stabilization effect of (NH₄)₂SiF₆ treatment on the hydrothermal stability of mesoporous SBA-15 zeolite[J]. Chinese Journal of Catalysis, 2015, 36(7): 1001-1008.

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Al³⁺离子介入提升(NH₄)₂SiF₆对SBA-15介孔材料的水热稳定化作用

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

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