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Surface interaction and dynamics of molecular spin-probes as guests in tailor-made organosilica, porous hosts for applications in chromatography.

分子自旋探针作为客体在定制的有机二氧化硅、色谱应用的多孔主体中的表面相互作用和动力学。

基本信息

批准号：
246351073
负责人：
Professor Dr. Sebastian Polarz
金额：
--
依托单位：
Arbeitsgruppe Physikalische und Biophysikalische Chemie
依托单位国家：
德国
项目类别：
Priority Programmes
财政年份：
2013
资助国家：
德国
起止时间：
2012-12-31 至 2017-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/246351073?language=en
关键词：
Surface interaction dynamics molecular spin

项目摘要

Mass transport in, trough and out of porous solids is a deciding factor in a number of applications in process engineering, e.g. chromatography. One has to consider a hierarchical process, spanning several orders of length- and time-scales. At the molecular scale, in the range of few nanometers and picoseconds, there is a complex interplay between guest-solvent and guest-surface interactions, and this determines directly the mobility of those guests inside the porous materials. A comprehensive and scale-spanning, experimentally underpinned understanding of the transport of dissolved molecular species inside (functionalized) porous matrices is pivotal for realizing porous solids designated for particular applications (e.g. chromatography) by design rather than by empiricism. However, it is very difficult to "spot" the confined guests with sufficient temporal and spatial resolution at technically relevant conditions (in the presence of solvents and at T >= r.t.). We have successfully established electron spin resonance (ESR) spectroscopy as an analytical "eye". Now, we will advance the ESR methodology, aiming at more precise and first and foremost scale-spanning insights into the diffusion of molecular spin probes in pores. Furthermore, we are going to establish a direct link between the synthesis of tailor-made, porous materials, which will enable to exert a much more controlled influence on the mass transport of dissolved species. We will dedicate ourselves to the exciting question of effects of spectator groups, which are present in addition to the active components (predominantly taking part in the guest-surface interaction). We expect that the mobility of guest molecules is mainly dependent on the surface density of the active components, but spectator groups may have a significant importance as well due to the local affect on solvent properties, for instance. The required, systematic variations of surface properties will be realized via bifunctional organosilica materials. Due to the high degree of novelty, we anticipate a substantial acquisition of new knowledge from the combination of materials with chemical gradients and imaging ESR spectroscopy. The imaging methodology allows recording the spectroscopic signature of the guests at every position of the porous material. From these data we can obtain information about the local dynamics and mobility, and at the same time one can analyse the mass transport through the porous medium at macroscopic dimensions. The direct correlation between molecular and macroscopic transport will finally enable to investigate the separation of a compound mixture, by means of spectroscopy using two different spin probes and also for the concrete application, a chromatographic measurement.

质量在多孔固体中进出是过程工程中许多应用的决定性因素，例如色谱。我们必须考虑一个分层的过程，跨越数个长度和时间尺度。在分子尺度上，在几纳米和皮秒的范围内，客体-溶剂和客体-表面相互作用之间存在复杂的相互作用，这直接决定了这些客体在多孔材料内的流动性。对溶解的分子物种在（功能化）多孔基质内的运输进行全面的、跨越规模的、实验基础的理解，对于通过设计而不是通过经验来实现指定用于特定应用（如色谱）的多孔固体是至关重要的。然而，在技术上相关的条件下（在溶剂存在和t> = r.t时），很难以足够的时间和空间分辨率“发现”受限来宾。我们成功地建立了电子自旋共振（ESR）光谱作为分析的“眼睛”。现在，我们将推进ESR方法，旨在更精确地了解分子自旋探针在孔隙中的扩散。此外，我们将在定制的多孔材料的合成之间建立直接联系，这将使我们能够对溶解物质的质量传递施加更可控的影响。我们将致力于研究观众群体的影响这一令人兴奋的问题，除了积极的组成部分（主要是参与嘉宾与地面的互动）之外，观众群体也存在。我们预计客体分子的迁移率主要取决于活性组分的表面密度，但旁观者基团也可能具有显著的重要性，例如，由于对溶剂性质的局部影响。所需的、系统的表面特性变化将通过双功能有机二氧化硅材料来实现。由于高度的新颖性，我们期望从化学梯度和成像ESR光谱的材料组合中获得大量的新知识。成像方法允许在多孔材料的每个位置记录客人的光谱特征。从这些数据中我们可以得到有关局部动力学和迁移率的信息，同时也可以从宏观的角度分析质量在多孔介质中的输运。分子和宏观运输之间的直接关系将最终使我们能够通过使用两种不同的自旋探针的光谱学以及具体应用的色谱测量来研究化合物混合物的分离。

项目成果

期刊论文数量（7）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Localization of Guest Molecules in Nanopores by Pulsed EPR Spectroscopy

通过脉冲 EPR 光谱定位纳米孔中的客体分子

DOI：
10.1021/acs.jpcc.7b10758
发表时间：
2018
期刊：
Journal of Physical Chemistry C
影响因子：
3.7
作者：
A. Pivtsov;M. Wessig;V. Klovak;S. Polarz;M. Drescher
通讯作者：
M. Drescher

Negative and Positive Confinement Effects in Chiral Separation Chromatography Monitored with Molecular-Scale Precision by In-Situ Electron Paramagnetic Resonance Techniques.

通过原位电子顺磁共振技术以分子级精度监测手性分离色谱中的负限制效应和正限制效应

DOI：
10.1021/acs.langmuir.7b02713
发表时间：
2017
期刊：
Langmuir : the ACS journal of surfaces and colloids
影响因子：
0
作者：
M. Wessig;M. Spitzbarth;A. Klaiber;M. Drescher;S. Polarz
通讯作者：
S. Polarz

Directional Materials—Nanoporous Organosilica Monoliths with Multiple Gradients Prepared Using Click Chemistry.

DOI：
10.1002/anie.201502878
发表时间：
2015-09
期刊：
Angewandte Chemie
影响因子：
0
作者：
A. Schachtschneider;Martin Wessig;Martin Spitzbarth;A. Donner;C. Fischer;M. Drescher;S. Polarz
通讯作者：
A. Schachtschneider;Martin Wessig;Martin Spitzbarth;A. Donner;C. Fischer;M. Drescher;S. Polarz

Multiple scale investigation of molecular diffusion inside functionalized porous hosts using a combination of magnetic resonance methods.

使用磁共振方法组合对功能化多孔主体内的分子扩散进行多尺度研究