结合异核相关核磁共振和自旋扩散检测分子固体中Cl-H-H和N-H-H - h邻近值

IF 1.8 3区 化学 Q4 CHEMISTRY, PHYSICAL Solid state nuclear magnetic resonance Pub Date : 2022-08-01 DOI:10.1016/j.ssnmr.2022.101808
Parth Raval , Julien Trébosc , Tomasz Pawlak , Yusuke Nishiyama , Steven P. Brown , G.N. Manjunatha Reddy
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引用次数: 1

摘要

分析分子间的中短程相互作用为表征小分子和材料的固态组织提供了一种很好的方法。这可以通过二维(2D)同核和异核相关核磁共振波谱来实现,例如,通过在高磁场下与快速魔角旋转(MAS)技术相结合进行实验。但是,检测距离大于3 Å的异核偶极耦合自旋对的二维峰并不总是直截了当地,特别是当涉及低伽马四极核时。在这里,我们提出了一个二维相关核磁共振实验,结合了异核-多量子相干(HMQC)和基于质子的自旋扩散(SD)脉冲序列的优势,利用射频驱动补偿(RFDR)来探测分子间和分子内的1H-X (X = 14N, 35Cl)相互作用。本实验可获得经1H{X}-HMQC滤波后的二维1H- 1H相关光谱和二维1H-X HMQC光谱。采用二维HMQC-SD-RFDR方法,在高场(21.1 T和18.8 T)和快速MAS (60 kHz)下,对粉末形式的多巴胺·HCl和l-组氨酸·HCl·H2O进行了表征。固态核磁共振结果补充了核磁共振晶体学分析,使用包括投影仪增强波(GIPAW)方法。对于组氨酸·HCl·H2O,已检测到与14n - 1h和35cl - 1h距离达4.4和3.9 Å的2D峰。通过观察多巴胺·HCl中14n - 1h和35cl - 1h距离分别为4.2和3.7 Å的2D峰进一步证实了这一点,表明HMQC-SD-RFDR实验适用于检测分子固体中的中程距离。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Combining heteronuclear correlation NMR with spin-diffusion to detect relayed Cl–H–H and N–H–H proximities in molecular solids

Analysis of short-to-intermediate range intermolecular interactions offers a great way of characterizing the solid-state organization of small molecules and materials. This can be achieved by two-dimensional (2D) homo- and heteronuclear correlation NMR spectroscopy, for example, by carrying out experiments at high magnetic fields in conjunction with fast magic-angle spinning (MAS) techniques. But, detecting 2D peaks for heteronuclear dipolar coupled spin pairs separated by greater than 3 Å is not always straightforward, particularly when low-gamma quadrupolar nuclei are involved. Here, we present a 2D correlation NMR experiment that combines the advantages of heteronuclear-multiple quantum coherence (HMQC) and proton-based spin-diffusion (SD) pulse sequences using radio-frequency-driven-recouping (RFDR) to probe inter and intramolecular 1H-X (X = 14N, 35Cl) interactions. This experiment can be used to acquire 2D 1H{X}-HMQC filtered 1H–1H correlation as well as 2D 1H-X HMQC spectra. Powder forms of dopamine·HCl and l-histidine·HCl·H2O are characterized at high fields (21.1 T and 18.8 T) with fast MAS (60 kHz) using the 2D HMQC-SD-RFDR approach. Solid-state NMR results are complemented with NMR crystallography analyses using the gauge-including projector augmented wave (GIPAW) approach. For histidine·HCl·H2O, 2D peaks associated with 14N–1H–1H and 35Cl–1H–1H distances of up to 4.4 and 3.9 Å have been detected. This is further corroborated by the observation of 2D peaks corresponding to 14N–1H–1H and 35Cl–1H–1H distances of up to 4.2 and 3.7 Å in dopamine·HCl, indicating the suitability of the HMQC-SD-RFDR experiments for detecting medium-range proximities in molecular solids.

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来源期刊
CiteScore
5.30
自引率
9.40%
发文量
42
审稿时长
72 days
期刊介绍: The journal Solid State Nuclear Magnetic Resonance publishes original manuscripts of high scientific quality dealing with all experimental and theoretical aspects of solid state NMR. This includes advances in instrumentation, development of new experimental techniques and methodology, new theoretical insights, new data processing and simulation methods, and original applications of established or novel methods to scientific problems.
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