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SSZ-87:一种具有异常灵活的 10 元环孔开口的硼硅酸盐沸石。

SSZ-87: a borosilicate zeolite with unusually flexible 10-ring pore openings.

机构信息

Laboratory of Crystallography, ETH Zurich , Vladimir-Prelog-Weg 5, Zurich CH-8093, Switzerland.

出版信息

J Am Chem Soc. 2015 Feb 11;137(5):2015-20. doi: 10.1021/ja512411b. Epub 2015 Feb 2.

Abstract

The structure of the as-synthesized borosilicate zeolite SSZ-87 has been solved by combining high-resolution X-ray powder diffraction (XPD) and rotation electron diffraction (RED) techniques. The unit cell and space group symmetry were found from the XPD data, and were essential for the initial analysis of the RED data. Although the RED data were only 15% complete, this proved to be enough for structure solution with the program Focus. The framework topology is the same as that of ITQ-52 (IFW), but for SSZ-87 the locations of the structure directing agent (SDA) and the B atoms could also be determined. SSZ-87 has large cages interconnected by 8- and 10-rings. However, results of hydroisomerization and Al insertion experiments are much more in line with those found for 12-ring zeolites. This prompted the structure analyses of SSZ-87 after calcination, and Al insertion. During calcination, the material is also partially deboronated, and the location of the resulting vacancies is consistent with those of the B atoms in the as-synthesized material. After Al insertion, SSZ-87 was found to contain almost no B and to be defect free. In its calcined and deboronated form, the pore system of SSZ-87 is more flexible than those of other 10-ring zeolites. This can be explained by the fact that the large cages in SSZ-87 are connected via single rather than double 10-ring windows and that there are vacancies in some of these 10-rings.

摘要

采用高分辨率 X 射线粉末衍射(XPD)和旋转电子衍射(RED)技术相结合的方法,解析了合成的硼硅酸盐沸石 SSZ-87 的结构。从 XPD 数据中找到了晶胞和空间群对称性,这对于 RED 数据的初步分析是必不可少的。尽管 RED 数据仅完成了 15%,但这对于使用 Focus 程序进行结构解析已足够。骨架拓扑结构与 ITQ-52(IFW)相同,但对于 SSZ-87,可以确定结构导向剂(SDA)和 B 原子的位置。SSZ-87 由大笼通过 8-和 10-元环相互连接。然而,加氢异构化和 Al 插入实验的结果更符合 12-元环沸石的结果。这促使我们对 SSZ-87 进行了煅烧和 Al 插入后的结构分析。在煅烧过程中,材料也会部分脱硼,所得空位的位置与合成材料中 B 原子的位置一致。Al 插入后,SSZ-87 几乎不含 B 且无缺陷。在煅烧和脱硼形式下,SSZ-87 的孔系统比其他 10-元环沸石更灵活。这可以解释为 SSZ-87 中的大笼通过单而非双 10-元环窗口连接,并且这些 10-元环中的一些存在空位。

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