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使用设计的有机结构导向剂直接合成具有相交的12×11×11元环孔道的硅铝酸盐POS沸石。

Direct Synthesis of An Aluminosilicate POS Zeolite with Intersecting 12×11×11-Member-Ring Pore Channels by Using a Designed Organic Structure-Directing Agent.

作者信息

Cai Xianshu, Zhao Yue, Zhang Jun, Zi Wenwen, Tao Shuo, Jiao Feng, Du Hongbin

机构信息

State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023, P. R. China.

School of Materials and Chemical Engineering, Anhui Jianzhu University, Hefei, 230601, P.R. China.

出版信息

Chemistry. 2022 Jun 21;28(35):e202201075. doi: 10.1002/chem.202201075. Epub 2022 May 12.

Abstract

Large and extra-large pore zeolites have been widely applied in industrial areas as catalysts, adsorbents, etc. Among them, silica and/or aluminosilicate zeolites have been attracted great attention due to their excellent hydrothermal stability and strong acidity. However, a great deal of zeolite structures are still not available in the form of silica and/or aluminosilicate. Herein, we report the synthesis of pure silica and aluminosilicate large-pore zeolites, denoted as NUD-14 and Al-NUD-14, respectively, by using a designed cation 1-ethyl-4-phenylpyridinium as an organic structure-directing agent (OSDA). NUD-14 has an intersecting 12×11×11-member ring pore system, which is isostructural to the germanosilicate PUK-16 zeolite with a POS topology. The OSDAs can be completely removed from the framework by calcination. NUD-14 and Al-NUD-14 possess excellent acid and hydrothermal stabilities, superior to the germanosilicate POS zeolite. The incorporation of Al into the zeolite framework makes the Al-NUD-14 zeolite possess medium and strong acidities. The successful synthesis of NUD-14 consisting of a rare odd-member ring pore structure may provide a platform for interesting size- and shape-selective catalytic applications.

摘要

大孔和超大孔沸石已作为催化剂、吸附剂等在工业领域得到广泛应用。其中,硅铝酸盐沸石因其优异的水热稳定性和强酸性而备受关注。然而,许多沸石结构仍无法以硅铝酸盐的形式获得。在此,我们报道了通过使用设计的阳离子1-乙基-4-苯基吡啶鎓作为有机结构导向剂(OSDA),分别合成纯硅和硅铝酸盐大孔沸石,分别记为NUD-14和Al-NUD-14。NUD-14具有交叉的12×11×11元环孔系统,与具有POS拓扑结构的锗硅PUK-16沸石同构。通过煅烧可将OSDA从骨架中完全去除。NUD-14和Al-NUD-14具有优异的酸性和水热稳定性,优于锗硅POS沸石。将Al引入沸石骨架使Al-NUD-14沸石具有中强酸性。由罕见的奇元环孔结构组成的NUD-14的成功合成可能为有趣的尺寸和形状选择性催化应用提供一个平台。

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