改善SBA-15介孔材料水热稳定性的简单溶剂热后处理方法

doi:10.1016/S1872-2067(15)60857-9

催化学报 ›› 2015, Vol. 36 ›› Issue (8): 1350-1357.DOI: 10.1016/S1872-2067(15)60857-9

改善SBA-15介孔材料水热稳定性的简单溶剂热后处理方法

邹成龙^a, 沙观宇^b, 顾海芳^b, 黄曜^b, 牛国兴^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:2015-02-10 修回日期:2015-03-30 出版日期:2015-07-29 发布日期:2015-07-30
通讯作者: 牛国兴
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(20890123).

Facile solvothermal post-treatment to improve hydrothermal stability of mesoporous SBA-15 zeolite

Chenglong Zou^a, Guanyu Sha^b, Haifang Gu^b, Yao Huang^b, Guoxing Niu^a

a Department of Chemistry, Fudan University, Shanghai 200433, China;
b Department of Materials Science, Fudan University, Shanghai 200433, China

Received:2015-02-10 Revised:2015-03-30 Online:2015-07-29 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 (20890123).

摘要/Abstract

摘要：

提出了一种有效改善SBA-15介孔材料水热稳定性的简单溶剂热后处理方法. SBA-15材料经环己烷、甲苯和正丁醇等有机溶剂在157和190 ℃密闭容器中分别处理6-24 h后, 可呈现很好的水热稳定性. 它们在800 ℃经100%水蒸气处理12 h, 依然能保持很好的有序介孔结构, 比表面积可高达192-281 m²/g. 其中, 经环己烷190 ℃溶剂热处理24 h的样品表现出最优的水热稳定性. 溶剂热处理能显著提升材料孔壁中类似Si(OSi)₂(OH)₂和Si(OSi)₃OH结构的Si-OH基间脱水, 形成稳定的Si(OSi)₄结构, 从而有效减少了SBA-15材料孔壁的缺陷. 由此, 介孔材料的水热稳定性得到明显改善. 溶剂热处理对SBA-15材料水热稳定性的这种提升作用与所用溶剂性质、处理温度以及SBA-15前驱体的类型密切相关. 其中, 以低沸点的非极性溶剂处理焙烧后的SBA-15材料表现出最好的稳定化效果. 该方法具有简单、低能耗的特点, 其在制备高水热稳定的有序硅基介孔材料上有很好的潜在应用价值.

关键词: 介孔材料, SBA-15分子筛, 水热稳定性, 溶剂热处理, 脱水

Abstract:

A simple and effective approach is demonstrated to improve the hydrothermal stability of mesoporous SBA-15 zeolite via a post-synthesis treatment of organic solvents, such as cyclohexane, toluene and n-butanol, at 157 or 190 ℃ for 6-24 h. After hydrothermal treatment at 800 ℃ for 12 h in 100% steam, the treated SBA-15 retained a well-ordered mesostructure, and retained high surface areas of 192-281 m²/g. SBA-15 zeolite treated by cyclohexane at 190 ℃ for 24 h showed the highest hydrothermal stability. The stabilization mechanism suggests that the solvothermal treatment has a significant promoting effect on dehydrating Si-OH groups in silica walls to form stable Si(OSi)₄ from Si(OSi)₂(OH)₂ or Si(OSi)₃OH groups. As a result, the wall defects after solvothermal treatment decrease, and the stability of silica is improved remarkably. This promoting effect strongly depends on the solvent properties, treatment temperature, and precursors of SBA-15 zeolite. The treatment by a nonpolar and low boiling point organic solvent displays the highest promoting effect on the calcined SBA-15 zeolite. This approach is simple, has low energy consumption and has potential application in the laboratory and for industry to prepare hydrothermally stable well-ordered mesoporous SBA-15 zeolite.

Key words: Mesoporous material, SBA-15 zeolite, Hydrothermal stability, Solvothermal treatment, Dehydration

邹成龙, 沙观宇, 顾海芳, 黄曜, 牛国兴. 改善SBA-15介孔材料水热稳定性的简单溶剂热后处理方法[J]. 催化学报, 2015, 36(8): 1350-1357.

Chenglong Zou, Guanyu Sha, Haifang Gu, Yao Huang, Guoxing Niu. Facile solvothermal post-treatment to improve hydrothermal stability of mesoporous SBA-15 zeolite[J]. Chinese Journal of Catalysis, 2015, 36(8): 1350-1357.

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改善SBA-15介孔材料水热稳定性的简单溶剂热后处理方法

Facile solvothermal post-treatment to improve hydrothermal stability of mesoporous SBA-15 zeolite

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