4.5 Article

Temperature-Dependent Solid-State NMR Proton Chemical-Shift Values and Hydrogen Bonding

期刊

JOURNAL OF PHYSICAL CHEMISTRY B
卷 125, 期 23, 页码 6222-6230

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcb.1c04061

关键词

-

资金

  1. ETH Research Grant [ETH-43 17-2]
  2. Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [455240421]
  3. Heisenberg fellowship
  4. ERC Advanced Grant [741863]
  5. Swiss National Science Foundation [200020_159707, 200020-188711]
  6. ANRS [ECTZ100488, ECTZ71388]
  7. ANR [ANR-19-CE11-0023]
  8. European Research Council (ERC) [741863] Funding Source: European Research Council (ERC)

向作者/读者索取更多资源

This study demonstrates that fast temporal stabilization of a magnetic field is achievable by actively stabilizing the temperature of the magnet bore. It allows quantification of the weak temperature dependence of proton chemical shift, which is diagnostic for hydrogen bond presence. Hydrogen bonding plays a crucial role in molecular recognition events, however, direct detection remains challenging due to resolution limitations.
Temperature-dependent NMR experiments are often complicated by rather long magnetic-field equilibration times, for example, occurring upon a change of sample temperature. We demonstrate that the fast temporal stabilization of a magnetic field can be achieved by actively stabilizing the temperature of the magnet bore, which allows quantification of the weak temperature dependence of a proton chemical shift, which can be diagnostic for the presence of hydrogen bonds. Hydrogen bonding plays a central role in molecular recognition events from both fields, chemistry and biology. Their direct detection by standard structure-determination techniques, such as X-ray crystallography or cryo-electron microscopy, remains challenging due to the difficulties of approaching the required resolution, on the order of 1 A. We, herein, explore a spectroscopic approach using solid-state NMR to identify protons engaged in hydrogen bonds and explore the measurement of proton chemical-shift temperature coefficients. Using the examples of a phosphorylated amino acid and the protein ubiquitin, we show that fast magic-angle spinning (MAS) experiments at 100 kHz yield sufficient resolution in proton-detected spectra to quantify the rather small chemical-shift changes upon temperature variations.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.5
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

暂无数据
暂无数据