Jung Hye Ja, Shin Chae-Ho, Hong Suk Bong
Division of Chemical Engineering, Hanbat National University, Taejon 305-719, Korea.
J Phys Chem B. 2005 Nov 10;109(44):20847-53. doi: 10.1021/jp054199j.
The solid-state NMR evidence that Si atoms are not randomly distributed in microporous SAPO-35 materials with the LEV topology and their distribution is governed by the Si content in synthesis mixtures is presented. It is also shown that the extraction pattern of Si atoms from the two distinct tetrahedral sites of the SAPO-35 framework during the calcination step at elevated temperatures occurs in a nonrandom manner, which can be rationalized by considering the expected strain on each topologically distinct site. The overall results of this study reveal that, when the level of Si substitution in SAPO-35 materials is high enough to produce various heterogeneous Si environments other than Si(4Al) species having P atoms only as second-nearest T-atom neighbors, the oxide composition of the domain preferentially created is aluminosilicate rather than pure silica in nature.
本文给出了固态核磁共振证据,表明硅原子并非随机分布在具有LEV拓扑结构的微孔SAPO-35材料中,其分布受合成混合物中硅含量的控制。研究还表明,在高温煅烧步骤中,硅原子从SAPO-35骨架的两个不同四面体位置的萃取模式并非随机发生,通过考虑每个拓扑不同位置上预期的应变可以对此进行合理解释。这项研究的总体结果表明,当SAPO-35材料中的硅取代水平足够高,能够产生除了仅以磷原子作为第二近邻T原子的Si(4Al)物种之外的各种非均匀硅环境时,优先形成的区域的氧化物组成本质上是铝硅酸盐而非纯二氧化硅。