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通过超快魔角旋转提高动态核极化效率。

Dynamic Nuclear Polarization Efficiency Increased by Very Fast Magic Angle Spinning.

机构信息

Institut de Sciences Analytiques, Centre de RMN à Très Hauts Champs, Université de Lyon (CNRS/ENS Lyon/UCB Lyon 1), 69100 Villeurbanne, France.

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

出版信息

J Am Chem Soc. 2017 Aug 9;139(31):10609-10612. doi: 10.1021/jacs.7b05194. Epub 2017 Jul 27.

Abstract

Dynamic nuclear polarization (DNP) has recently emerged as a tool to enhance the sensitivity of solid-state NMR experiments. However, so far high enhancements (>100) are limited to relatively low magnetic fields, and DNP at fields higher than 9.4 T significantly drops in efficiency. Here we report solid-state Overhauser effect DNP enhancements of over 100 at 18.8 T. This is achieved through the unexpected discovery that enhancements increase rapidly with increasing magic angle spinning (MAS) rates. The measurements are made using 1,3-bisdiphenylene-2-phenylallyl dissolved in o-terphenyl at 40 kHz MAS. We introduce a source-sink diffusion model for polarization transfer which is capable of explaining the experimental observations. The advantage of this approach is demonstrated on mesoporous alumina with the acquisition of well-resolved DNP surface-enhanced Al cross-polarization spectra.

摘要

动态核极化 (DNP) 最近已成为提高固态 NMR 实验灵敏度的一种工具。然而,到目前为止,高增强 (>100) 仅限于相对较低的磁场,并且磁场高于 9.4 T 时 DNP 的效率会显著下降。在这里,我们报告了在 18.8 T 下超过 100 的固态 Overhauser 效应 DNP 增强。这是通过一个意外的发现实现的,即增强随着魔角旋转 (MAS) 速率的增加而迅速增加。该测量使用溶解在 o-三联苯中的 1,3-双二苯乙烯-2-苯丙烯在 40 kHz MAS 下进行。我们引入了一种用于极化转移的源-汇扩散模型,该模型能够解释实验观察结果。该方法的优势在介孔氧化铝上得到了证明,获得了分辨率良好的 DNP 表面增强 Al 交叉极化光谱。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5137/5719465/e6bff2da7bd1/ja-2017-051949_0001.jpg

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