Ionic Liquids in the Synthesis and Tuning of Porous Materials: Knowledge-based Design of Properties Using a Combined Experimental and Theoretical Approach

离子液体在多孔材料的合成和调节中：采用实验和理论相结合的方法进行基于知识的性能设计

• 批准号: 253301413
• 负责人: Professorin Dr. Barbara Kirchner
• 金额: --
• 依托单位: Mulliken Center for Theoretical Chemistry
• 依托单位国家: 德国
• 项目类别: Priority Programmes
• 财政年份: 2014
• 资助国家: 德国
• 起止时间: 2013-12-31 至 2018-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/253301413?language=en
• 关键词: Ionic; Liquids; Synthesis; Tuning; Porous

This project is a bilateral project between PD Dr. Annegret Stark (Leibniz-Institute of Surface Modification, Leipzig) and Prof. Dr. Barbara Kirchner (Universität Bonn). The expertise of experimentalists and theoreticians is hence combined. Research focus 1 (RF 1) of this project is concerned with the investigation of ionic liquids (ILs) as solvents and structure-directing agents in the synthesis of zeolites. It is the goal to understand the prevailing and governing interactions on molecular level, contributing to an understanding of the solvation and crystallisation mechanism leading to high selectivities in the resulting framework geometry. RF 2 investigates the properties of ILs in confinement, i.e. in porous materials. The aim is to provide a detailed knowledge of the interfacial structure and interactions between porous inorganic materials and ILs, leading to deviations from bulk liquid properties (density, melting point etc.). Investigations will be carried out systematically, including series of homologues of ILs where the cation, the anion or the cation substituent are successively altered. In RF 1, we will extend our prior studies from AlPOs to SAPOs, MAPOs and finally to true zeolites (aluminosilicates), to shed light into the limits of ionothermal zeolite synthesis regarding precursors, ionic liquid types and resulting framework types.In RF 2, we will investigate the properties and orientation of the IL in confinement in dependence of the ionic liquid structure (homologues series), the nature of the support (pore size, geometry, chemical composition) and the ionic liquid loading. Furthermore, the pore filling mechanism with respect to the type of support will be studied.The following research questions are in the centre of the project:1. Which structural features of the IL (type of cation, cation substituent, type of anion) affect the resulting framework type? Which interaction types prevail? 2. Can the IL be designed to generate new framework structures?3. What is the role of the mineralizer and can it be substituted by an IL function?4. Can the (low pressure) ionothermal synthesis be converted in a continuous synthesis protocol?5. What is the effect of the confinement on the physicochemical properties of the IL?6. How does the confinement affect the orientation of the IL?7. How does the IL constitution (i.e. its anion, cation, cation substituent) affect the orientation in confinement, compared to the bulk liquid?8. Is the pore filling mechanism dependent on the IL?

该项目是由Annegret Stark博士(莱布尼茨表面改性研究所，莱比锡)和Barbara Kirchner教授(波恩大学)之间的双边项目。因此，实验学家和理论家的专业知识被结合在一起。本项目的研究重点1(Rf1)是关于离子液体(ILS)在合成沸石中作为溶剂和结构导向剂的研究。其目的是在分子水平上了解普遍存在的和支配的相互作用，有助于理解溶剂化和结晶机制导致所得到的框架几何图形中的高选择性。RF2研究了离子液体在约束条件下的性质，即在多孔材料中的性质。其目的是提供关于多孔无机材料与离子液体之间的界面结构和相互作用的详细知识，从而导致与大块液体性质(密度、熔点等)的偏差。将进行系统的研究，包括一系列离子液体的同系物，其中阳离子、阴离子或阳离子取代基连续改变。在Rf1中，我们将把我们先前的研究从Alpos扩展到Sapos、MAPOS，最后扩展到真正的沸石(铝硅酸盐)，以揭示离子热沸石合成的限制条件，包括前驱体、离子液体类型和生成的骨架类型。在Rf2中，我们将研究离子液体结构(同系物系列)、载体的性质(孔大小、几何形状、化学组成)和离子液体负载量对离子液体限制的性质和取向的影响。此外，还将研究与载体类型有关的孔填充机制。本项目的中心研究问题如下：1.IL(阳离子类型、阳离子取代基、阴离子类型)的哪些结构特征影响所得到的骨架类型？哪种相互作用类型占优势？2.IL能被设计成产生新的骨架结构吗？3.矿化剂的作用是什么？它能被IL功能取代吗？4.(低压)离子热合成能在连续合成方案中转化吗？5.限制对IL的物理化学性质有什么影响？6.限制对IL的取向有何影响？7.与大块液体相比，IL的组成(即其阴离子、阳离子、阳离子取代基)如何影响限制中的取向？8.孔填充机制依赖于IL吗？