Division of Materials Science and Chemical Engineering, Yokohama National University , 79-5 Tokiwadai, Hodogaya-ku, Yokohama 240-8501, Japan.
National Institute of Advanced Industrial Science and Technology , 4-2-1 Nigatake, Miyagino-ku, Sendai 983-8551, Japan.
J Am Chem Soc. 2017 Jun 14;139(23):7989-7997. doi: 10.1021/jacs.7b03308. Epub 2017 Jun 5.
Synthesis of new zeolites with controlled pore architectures is important in the field of catalysis and separation related to chemical transformation, environmental protection, and energy-saving. Zeolites containing channels of different sizes in the same framework have been desirable. We report here the synthesis and structure of a novel aluminosilicate zeolite (designated as YNU-5), the first zeolite containing interconnected 12-, 12-, and 8-ring pores, as well as independent straight 8-ring channels. The synthesis procedure is quite simple and consists of conventional hydrothermal conditions as well as readily available starting materials. The framework structure is stable enough and Si/Al ratio is controllable between 9 and 350. Determination of the crystal structure is performed by utilizing X-ray diffraction-based techniques, revealing 9 independent tetrahedrally coordinated atoms. This robust structure is expected to be industrially valuable and several unusual combinations of composite building units are of considerable interest in an academic sense. The new zeolite YNU-5 is promising catalyst for the production of useful light olefins such as propylene and butylenes in the dimethyl ether-to-olefin reaction, when the Si/Al ratio is properly tuned by dealumination through simple acid treatments.
具有可控孔结构的新型沸石的合成在与化学转化、环境保护和节能相关的催化和分离领域非常重要。在同一骨架中具有不同尺寸通道的沸石一直是人们所期望的。我们在这里报告了一种新型铝硅酸盐沸石(命名为 YNU-5)的合成和结构,这是第一种含有相互连接的 12-、12-和 8-元环孔以及独立的直 8-元环通道的沸石。该合成方法非常简单,包括常规的水热条件以及易于获得的起始材料。骨架结构足够稳定,Si/Al 比可在 9 到 350 之间控制。通过利用基于 X 射线衍射的技术来确定晶体结构,揭示了 9 个独立的四面体配位原子。这种坚固的结构有望在工业上具有价值,并且一些不寻常的复合构建单元的组合在学术上具有相当大的兴趣。当通过简单的酸处理通过脱铝作用适当调整 Si/Al 比时,新型沸石 YNU-5 是在二甲醚制烯烃反应中生产有用的轻烯烃(如丙烯和丁烯)的有前途的催化剂。