Single-Scan Diffusion-Ordered NMR Spectroscopy of SABRE-Hyperpolarized Mixtures
Single-Scan Diffusion-Ordered NMR Spectroscopy of SABRE-Hyperpolarized Mixtures
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DOI：
10.1002/cphc.201800983
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发表时间：
2019-02-04
期刊：
影响因子：
2.9
通讯作者：
Huber, Gaspard
中科院分区：
文献类型：
--
作者：
Guduff, Ludmilla;Berthault, Patrick;Huber, Gaspard
对溶解分子的复杂混合物的分析是一个主要的挑战，特别是对于逐渐演化的系统，例如在化学反应过程中或在化学不稳定的情况下。一维核磁共振是一种快速、非侵入性的方法，适用于详细的分子分析，但灵敏度较低。此外，核磁共振中最常用、最灵敏的稳定同位素质子的光谱分辨率也相当有限。空间编码(SPEN)实验旨在通过在核磁共振管的不同切片上同时执行不同的一维子实验，以额外的灵敏度损失为代价，在一次采集中创建2D数据集。选择平移扩散系数作为附加维度(所谓的剂量法)有助于恢复混合物中每个分子的质子光谱。另一方面，SPEN核磁共振的灵敏度限制可以用超极化方法来解决。在超极化方法中，基于仲氢的可逆交换信号放大(SABRE)是最便宜、最容易建立的方法，并且允许多次实验。在这里，我们展示了通过结合SABRE、SPEN和剂量概念，在几秒钟内就能分辨出毫摩尔浓度下混合物组分的光谱。
The analysis of complex mixtures of dissolved molecules is a major challenge, especially for systems that gradually evolve, e. g., in the course of a chemical reaction or in the case of chemical instability. 1D NMR is a fast and non-invasive method suitable for detailed molecular analysis, though of low sensitivity. Moreover, the spectral resolution of proton, the most commonly used and most sensitive stable isotope in NMR, is also quite limited. Spatially encoded (SPEN) experiments aim at creating in one acquisition a 2D data set by simultaneously performing different 1D sub-experiments on different slices of the NMR tube, at the price of an extra loss of sensitivity. Choosing translational diffusion coefficients as the additional dimension (the so-called DOSY approach) helps to recover proton spectra of each molecule in a mixture. The sensitivity limitation of SPEN NMR can, on the other hand, be addressed with hyperpolarization methods. Within hyperpolarization methods, signal amplification by reversible exchange (SABRE), based on parahydrogen, is the cheapest and the easiest one to set up, and allows multi-shot experiments. Here we show that the spectra of a mixture's components at millimolar concentration are resolved in few seconds by combining the SABRE, SPEN and DOSY concepts.