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现成的硝酸钆作为用于魔角旋转动态核极化的高效高自旋金属离子极化剂。

Off-the-Shelf Gd(NO) as an Efficient High-Spin Metal Ion Polarizing Agent for Magic Angle Spinning Dynamic Nuclear Polarization.

作者信息

Elliott Stuart J, Duff Benjamin B, Taylor-Hughes Ashlea R, Cheney Daniel J, Corley John P, Paul Subhradip, Brookfield Adam, Pawsey Shane, Gajan David, Aspinall Helen C, Lesage Anne, Blanc Frédéric

机构信息

Department of Chemistry, University of Liverpool, Liverpool L69 7ZD, United Kingdom.

Stephenson Institute for Renewable Energy, University of Liverpool, Liverpool L69 7ZD, United Kingdom.

出版信息

J Phys Chem B. 2022 Aug 25;126(33):6281-6289. doi: 10.1021/acs.jpcb.2c04184. Epub 2022 Aug 16.

Abstract

Magic angle spinning nuclear magnetic resonance spectroscopy experiments are widely employed in the characterization of solid media. The approach is incredibly versatile but deleteriously suffers from low sensitivity, which may be alleviated by adopting dynamic nuclear polarization methods, resulting in large signal enhancements. Paramagnetic metal ions such as Gd have recently shown promising results as polarizing agents for H, C, and N nuclear spins. We demonstrate that the widely available and inexpensive chemical agent Gd(NO) achieves significant signal enhancements for the C and N nuclear sites of [2-C,N]glycine at 9.4 T and ∼105 K. Analysis of the signal enhancement profiles at two magnetic fields, in conjunction with electron paramagnetic resonance data, reveals the solid effect to be the dominant signal enhancement mechanism. The signal amplification obtained paves the way for efficient dynamic nuclear polarization without the need for challenging synthesis of Gd polarizing agents.

摘要

魔角旋转核磁共振光谱实验广泛应用于固体介质的表征。该方法用途极为广泛,但令人遗憾的是灵敏度较低,采用动态核极化方法可缓解这一问题,从而实现大幅信号增强。诸如钆(Gd)等顺磁性金属离子最近作为氢、碳和氮核自旋的极化剂显示出了有前景的结果。我们证明,广泛可得且价格低廉的化学试剂硝酸钆(Gd(NO))在9.4特斯拉和~105开尔文的条件下,能使[2 - C,N]甘氨酸的碳和氮核位点实现显著的信号增强。对两个磁场下的信号增强谱进行分析,并结合电子顺磁共振数据,表明固体效应是主要的信号增强机制。所获得的信号放大为高效动态核极化铺平了道路,而无需进行具有挑战性的钆极化剂合成。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1cf9/9421651/7cab18e4d0d2/jp2c04184_0001.jpg

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