α-d-葡萄糖两种形态氢键的固体核磁共振结合量子化学计算研究

IF 1.8 3区 化学 Q4 CHEMISTRY, PHYSICAL Solid state nuclear magnetic resonance Pub Date : 2023-02-01 DOI:10.1016/j.ssnmr.2022.101848
Darren H. Brouwer, Janelle G. Mikolajewski
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引用次数: 1

摘要

氢键在各种材料的结构和功能中起着重要作用。固态1H核磁共振(NMR)光谱为研究氢键中氢原子的局部结构提供了一种非常灵敏的工具。虽然有大量关于固体羧酸中O–H-O氢键的1H固态NMR数据,但还没有对碳水化合物中的羟基(以及一般的羟基)进行系统的1H固体NMR研究。为了研究更复杂材料(如纤维素多晶型物)中的氢键,我们对模型化合物α-d-葡萄糖和α-d-葡糖一水合物进行了详细的固态1H NMR研究。通过快速魔角自旋(MAS)、组合旋转和多脉冲光谱(CRAMPS)以及在超高磁场下进行的二维(2D)相关实验的组合,可以确定两种形式的α-d-葡萄糖中的所有脂族(CH)、羟基(OH)和水(H2O)的1H化学位移。采用平面波DFT计算来改善α-d-葡萄糖一水合物的氢原子位置,并计算1H化学位移,为实验确定的峰分配提供了额外的支持。最后,研究了羟基1H化学位移与其氢键几何结构之间的关系,并将其与羧酸质子的公认关系进行了比较。
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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A combined solid-state NMR and quantum chemical calculation study of hydrogen bonding in two forms of α-d-glucose

Hydrogen bonding plays an important role in the structure and function of a wide range of materials. Solid-state 1H nuclear magnetic resonance (NMR) spectroscopy provides a very sensitive tool to investigate the local structure of hydrogen atoms involved in hydrogen bonding. While there is extensive 1H solid-state NMR data on O–H - - O hydrogen bonding in solid carboxylic acids, there has been no systematic 1H solid-state NMR studies of hydroxyl groups in carbohydrates (and hydroxyl groups in general). With a view to studying the hydrogen bonding in more complex materials such as cellulose polymorphs, we carried out a detailed solid-state 1H NMR investigation of the model compounds α-d-glucose and α-d-glucose monohydrate. Through a combination of fast magic-angle spinning (MAS), combined rotation and multiple pulse spectroscopy (CRAMPS), and two-dimensional (2D) correlation experiments carried out at ultrahigh magnetic fields, it was possible to assign all of the aliphatic (CH), hydroxyl (OH), and water (H2O) 1H chemical shifts in both forms of α-d-glucose. Plane-wave DFT calculations were employed to improve the hydrogen atom positions for α-d-glucose monohydrate and to calculate 1H chemical shifts, providing additional support for the experimentally determined peak assignments. Finally, the relationship between the hydroxyl 1H chemical shifts and their hydrogen bonding geometry was investigated and compared to the well-established relationship for carboxylic acid protons.

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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.
期刊最新文献
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