Steam Stable Mesoporous Silica MCM-41 Stabilized by Trace Amounts of Al

被引:28
作者
Tompkins, Jordan T. [1 ]
Mokaya, Robert [1 ]
机构
[1] Univ Nottingham, Nottingham NG7 2RD, England
关键词
mesoporous silica MCM-41; alumination; steam stability; Al-grafted MCM-41; dry grafting; Al content; Si/Al ratio; HYDROTHERMAL STABILITY; MOLECULAR-SIEVES; ALUMINOSILICATE MESOSTRUCTURES; ENHANCED STABILITY; CATALYTIC-ACTIVITY; TETRAHEDRAL SITES; ION-EXCHANGE; ALUMINATION; IMPROVEMENT; ACIDITY;
D O I
10.1021/am404911x
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Evaluation of low and ultralow Al content (Si/Al between 50 and 412) aluminosilicate Al-MCM-41 materials synthesized via three contrasting alumination routes, namely, direct mixed-gel synthesis, post-synthesis wet grafting, and post-synthesis dry grafting, indicates that trace amounts of Al introduced via dry grafting can stabilize mesoporous silica MCM-41 to steaming at 900 degrees C for 4 h. It was found that trace amounts of Al (Si/Al > 400) introduced via so-called dry grafting of Al stabilize the virtually F purely siliceous MCM-41 to steaming, whereas Al incorporated via other methods that involve aqueous media such as direct mixed gel synthesis or wet grafting of Al offer only limited protection at low Al content. It is particularly remarkable that a post-synthesis dry grafted Al-MCM-41 material possessing trace amounts of Al (i.e., Si/Al ratio of 412) and surface area and pore volume of 1112 m(2)/g and 1.20 cm(3)/g respectively, retains 90% (998 m(2)/g) of the surface area and 85% (1.03 cm(3)/g) of the pore volume after exposure to steaming at 900 degrees C for 4 h. Under similar steam treatment conditions, the mesostructure of pure silica Si-MCM-41 is virtually destroyed and undergoes a 93% reduction in surface area (958 m(2)/g to 69 m(2)/g) and 88% decrease in pore volume (0.97 cm(3)/g to 0.12 cm(3)/g). The steam stable ultralow (i.e., trace) Al containing MCM-41 materials is found to be virtually similar to mesoporous pure silica Si-MCM-41 with hardly any detectable acidity. The improvement in steam stability arises from not only the presence of trace amounts of Al, but also from an apparent increase in the level of silica condensation that is specific to dry grafted alluminosilicate MCM-41 materials. The more highly condensed framework has fewer silanol groups and therefore is more resistant to hydrolysis under steaming conditions.
引用
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页码:1902 / 1908
页数:7
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