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使用小咪唑阳离子作为有机结构导向剂合成超大孔、大孔和中孔沸石

Synthesis of Extra-Large Pore, Large Pore and Medium Pore Zeolites Using a Small Imidazolium Cation as the Organic Structure-Directing Agent.

作者信息

Gao Zihao Rei, Balestra Salvador R G, Li Jian, Camblor Miguel A

机构信息

Instituto de Ciencia de Materiales de Madrid, Consejo Superior de Investigaciones Científicas (ICMM-CSIC), c/ Sor Juana Inés de la Cruz, 3, Madrid, 28049, Spain.

Berzelii Center EXSELENT on Porous Materials, Department of Materials and Environmental Chemistry, Stockholm University, Stockholm, 10691, Sweden.

出版信息

Chemistry. 2021 Dec 23;27(72):18109-18117. doi: 10.1002/chem.202103288. Epub 2021 Nov 17.

DOI:10.1002/chem.202103288
PMID:34730258
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9299198/
Abstract

One common strategy in the search for new zeolites is the use of organic structure-directing agents (OSDA). Typically, one seeks to achieve a high specificity in the structure-directing effect of the OSDA. This study shows, however, that an OSDA lacking strong specificity towards any particular zeolite may provide opportunities for discovery when other synthesis parameters are systematically screened. Thus, 1-methyl-2-ethyl-3-n-propylimidazolium has allowed to crystallize the new large/medium pore zeolite HPM-16 as well as the recently reported extra-large pore -SYT and the medium/small pore and chiral STW. The sophisticated OSDA originally affording -SYT and the new simple OSDA have very little in common, both in terms of size, shape and flexibility, while both may still direct the synthesis of the same zeolite. In fact, molecular simulations show that the new OSDA is located in three different positions of the -SYT structure, including the discrete 8MR where the original organic could not fit.

摘要

寻找新型沸石的一种常见策略是使用有机结构导向剂(OSDA)。通常,人们试图在OSDA的结构导向作用中实现高特异性。然而,这项研究表明,当系统地筛选其他合成参数时,对任何特定沸石缺乏强特异性的OSDA可能会提供发现的机会。因此,1-甲基-2-乙基-3-正丙基咪唑鎓已使新型大/中孔沸石HPM-16以及最近报道的超大孔-SYT和中/小孔及手性STW得以结晶。最初生成-SYT的复杂OSDA和新的简单OSDA在尺寸、形状和柔韧性方面几乎没有共同之处,而两者仍可能指导相同沸石的合成。事实上,分子模拟表明,新的OSDA位于-SYT结构的三个不同位置,包括原始有机物无法适配的离散8元环处。

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本文引用的文献

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HPM-16, a Stable Interrupted Zeolite with a Multidimensional Mixed Medium-Large Pore System Containing Supercages.HPM-16,一种具有包含超大笼的多维混合中-大孔系统的稳定介孔沸石。
Angew Chem Int Ed Engl. 2021 Sep 6;60(37):20249-20252. doi: 10.1002/anie.202106734. Epub 2021 Aug 9.
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Structure-direction towards the new large pore zeolite NUD-3.结构导向新型大孔沸石 NUD-3。
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HPM-14: A New Germanosilicate Zeolite with Interconnected Extra-Large Pores Plus Odd-Membered and Small Pores*.
HPM-14:一种具有相互连通的超大孔以及奇数元孔和小孔的新型锗硅酸盐沸石*
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Automated exploration of the low-energy chemical space with fast quantum chemical methods.运用快速量子化学方法探索低能量化学空间。
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Synthesis of a germanosilicate zeolite HPM-12 using a short imidazolium-based dication: structure-direction by charge-to-charge distance matching.使用短咪唑基二阳离子合成锗硅酸盐 HPM-12:通过电荷-电荷距离匹配的结构导向。
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Targeted Synthesis of a Zeolite with Pre-established Framework Topology.具有预先确定骨架拓扑结构的沸石的定向合成。
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Rediscovery of the Importance of Inorganic Synthesis Parameters in the Search for New Zeolites.重新发现无机合成参数在寻找新型沸石中的重要性。
Acc Chem Res. 2019 May 21;52(5):1419-1427. doi: 10.1021/acs.accounts.9b00073. Epub 2019 Apr 23.
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Exploration of Chemical Compound, Conformer, and Reaction Space with Meta-Dynamics Simulations Based on Tight-Binding Quantum Chemical Calculations.基于紧束缚量子化学计算的元动力学模拟对化合物、构象异构体和反应空间的探索
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GFN2-xTB-An Accurate and Broadly Parametrized Self-Consistent Tight-Binding Quantum Chemical Method with Multipole Electrostatics and Density-Dependent Dispersion Contributions.GFN2-xTB 一种精确且广泛参数化的自洽紧束缚量子化学方法,具有多极静电和密度相关色散贡献。
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