Application of NMR spectroscopy for the investigation of structure-mobility relations in nanoporous host-guest systems in concerted action with IR Micro-Imaging

核磁共振波谱与红外显微成像协同作用研究纳米多孔主客体系统的结构-迁移关系

基本信息

批准号：
277602929
负责人：
Professor Dr. Jürgen Haase
金额：
--
依托单位：
Abteilung Grenzflächenphysik
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2015
资助国家：
德国
起止时间：
2014-12-31 至 2019-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/277602929?language=en
关键词：
Application NMR spectroscopy investigation structure

项目摘要

With the focus on instrument-based and methodical work, in the course of the project KA 953/20-1,2, the background was set for new micro-imaging methods (measurement of transient concentration profiles with IR and interference microscopy). They provide a new approach to the exploration of molecular dynamics in nanoporous host-guest systems. NMR diffusometry with pulsed field gradients (PFG NMR) constitutes another microscopic method, which is complementary in a double fashion. First, it is applied under equilibrium conditions and, second, in the variation of temperature and pressure (and thereby of the guest loading) a much wider range can be covered (moreover, the variation is achieved with much less experimental effort). The potential offered by the concerted application of PFG NMR and Micro-Imaging shall be purposefully employed in this project to deepen our knowledge on molecular dynamics in nanoporous materials. The proposal is submitted in parallel with the application of C. Chmelik on "Micro-Imaging for the exploration of diffusion and reaction in nanoporous materials". A successful approach of the posed questions will be achieved only by the concerted use of both techniques. Besides technical and instrument-based developments for the use of PFG NMR in the particular fields (including the variation of temperature, pressure and observation time above the current limits), the work will be centered on the following three topics: (i) The combined measurement of self-diffusion (PFG NMR, this project) and transport diffusion (Micro-Imaging) establishes unprecedented options for the investigation of the interrelation of transport phenomena under equilibrium and non-equilibrium conditions. This is one of the fundamental questions of current research in the investigation of mesoscopic molecular systems under spatial confinement, which shall be in the focus of the studies within the first topic. (ii) We are, second, going to examine and to exploit the options of PFG NMR to study the impact of host-guest interactions on host structure and guest dynamics. This includes, in particular, the option of temperature variation over a wide range, in which drastic changes in the characteristics are expected. For the understanding of these processes and, possibly, even for their mere detection, a particular wide variation is essential. (iii) While the host-guest interactions considered in the second topic was found to give rise to a completely new type of hysteresis phenomena sorption hysteresis in mesoporous materials is known since over 100 years. However, the origin of this phenomenon and the intrinsic mechanisms determining its time dependence are still a topic of controversial discussion. With the information obtained by the combined application of PFG NMR and Micro-Imaging on the intrinsic dynamics of such systems we hope to contribute, within a third topic of our research plan, with so far inaccessible experimental evidence.

在项目KA 953/20-1,2的过程中，重点是基于仪器和有条不紊的工作，将背景设置为新的微成像方法（测量具有IR和干扰显微镜的瞬态浓度谱的测量）。它们为探索纳米多孔宿主 - 环系统中分子动力学的探索提供了新的方法。用脉冲场梯度（PFG NMR）的NMR扩散法构成了另一种显微镜方法，它以双重方式互补。首先，它在平衡条件下应用，其次，在温度和压力的变化（及其客人装载的变化）中可以覆盖更宽的范围（此外，通过减少实验性努力来实现这种变化）。 PFG NMR和微型成像的一致应用提供的潜力应有目的地利用，以加深我们对纳米多孔材料中分子动力学的了解。该提议与C. chmelik在“探索纳米多孔材料中扩散和反应的微观成像”上并行提交。提出问题的成功方法只能通过两种技术的一致使用来实现。 Besides technical and instrument-based developments for the use of PFG NMR in the particular fields (including the variation of temperature, pressure and observation time above the current limits), the work will be centered on the following three topics: (i) The combined measurement of self-diffusion (PFG NMR, this project) and transport diffusion (Micro-Imaging) establishes unprecedented options for the investigation of the interrelation of transport phenomena under平衡和非平衡条件。这是当前研究的基本问题之一，在空间限制下对介质分子系统的调查中，这应是第一个主题中的研究的重点。（ii）第二，我们将要检查并利用PFG NMR的选择来研究宿主 - 阵线相互作用对宿主结构和客体动态的影响。特别是，这包括温度变化在较大范围内的选择，其中预期特征的急剧变化。为了理解这些过程，甚至可能仅仅是为了发现它们，特定的广泛变化也是必不可少的。（iii）虽然第二个主题中考虑的宿主 - 阵线相互作用引起了介孔材料中一种全新类型的滞后现象滞后滞后，但自100多年以来就已经知道。但是，这种现象的起源和确定其时间依赖性的内在机制仍然是一个有争议的讨论的话题。通过通过PFG NMR的联合应用和微成像在我们希望在我们的研究计划的第三个主题中贡献的此类系统的固有动力学的合并应用获得的信息，到目前为止，迄今为止无法访问的实验证据。