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通过接力动态核极化对复杂粒子的径向分布函数进行成像。

Imaging Radial Distribution Functions of Complex Particles by Relayed Dynamic Nuclear Polarization.

机构信息

Institut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), Lausanne CH-1015, Switzerland.

Université de Bordeaux, CNRS, Bordeaux INP, ICMCB, UMR 5026, Pessac F-33600, France.

出版信息

J Am Chem Soc. 2023 May 3;145(17):9700-9707. doi: 10.1021/jacs.3c01279. Epub 2023 Apr 19.

Abstract

The physical properties of many modern multi-component materials are determined by their internal microstructure. Tools capable of characterizing complex nanoscale architectures in composite materials are, therefore, essential to design materials with targeted properties. Depending on the morphology and the composition, structures may be measured by laser diffraction, scattering methods, or by electron microscopy. However, it can be difficult to obtain contrast in materials where all the components are organic, which is typically the case for formulated pharmaceuticals, or multi-domain polymers. In nuclear magnetic resonance (NMR) spectroscopy, chemical shifts allow a clear distinction between organic components and can in principle provide the required chemical contrast. Here, we introduce a method to obtain radial images of the internal structure of multi-component particles from NMR measurements of the relay of nuclear hyperpolarization obtained from dynamic nuclear polarization. The method is demonstrated on two samples of hybrid core-shell particles composed of a core of polystyrene with a shell of mesostructured silica filled with the templating agent CTAB and is shown to yield accurate images of the core-shell structures with a nanometer resolution.

摘要

许多现代多组分材料的物理性质取决于其内部微观结构。因此,能够对复合材料中的复杂纳米结构进行特征化的工具对于设计具有目标性能的材料至关重要。根据形态和组成,可以通过激光衍射、散射方法或电子显微镜来测量结构。然而,在所有成分都是有机的情况下,获得对比度可能很困难,这通常是配方药物或多域聚合物的情况。在核磁共振(NMR)光谱中,化学位移可以在有机成分之间进行清晰区分,并可以在原则上提供所需的化学对比度。在这里,我们介绍了一种从动态核极化获得的核超极化接力的 NMR 测量中获取多组分颗粒内部结构的径向图像的方法。该方法在两个混合核壳粒子的样品上得到了验证,这些粒子由聚苯乙烯核和填充有模板剂 CTAB 的介孔二氧化硅壳组成,并显示出具有纳米分辨率的核壳结构的准确图像。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/da45/10760979/8c3b34e5d9c8/ja3c01279_0002.jpg

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