Highly Efficient Trityl-Nitroxide Biradicals for Biomolecular High-Field Dynamic Nuclear Polarization
Highly Efficient Trityl-Nitroxide Biradicals for Biomolecular High-Field Dynamic Nuclear Polarization
复制标题
用于生物分子高场动态核极化的高效三苯甲基氮氧双自由基
DOI：
10.1002/chem.202102253
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发表时间：
2021-07-22
影响因子：
4.3
通讯作者：
Liu, Yangping
中科院分区：
文献类型：
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作者：
Cai, Xinyi;Paioni, Alessandra Lucini;Liu, Yangping
动态核极化(DNP)是提高固体核磁共振(ss核磁共振)谱灵敏度的有效方法。然而，到目前为止，它在高磁场(最好是>；14T)下的生物分子应用一直受到极化剂和样品制备方面固有的低效率的限制。在这里，我们报道了一类新的三苯基-氮氧化物双自由基，称为SNAPol，它结合了高DNP效率和极大增强的亲水性。该系列中最好的化合物SNAPol-1在小分子和球状蛋白中显示出超过100的18.8T的DNP增强因子，在膜蛋白和细胞制剂中也显示出强烈的DNP增强作用。通过将最佳灵敏度和高分辨率相结合，我们期待这种新型偏振剂在高场DNP/单核磁共振光谱中得到广泛应用，特别是在复杂生物分子的研究中。
Dynamic nuclear polarization (DNP) is a powerful method to enhance the sensitivity of solid-state magnetic nuclear resonance (ssNMR) spectroscopy. However, its biomolecular applications at high magnetic fields (preferably>14 T) have so far been limited by the intrinsically low efficiency of polarizing agents and sample preparation aspects. Herein, we report a new class of trityl-nitroxide biradicals, dubbed SNAPols that combine high DNP efficiency with greatly enhanced hydrophilicity. SNAPol-1, the best compound in the series, shows DNP enhancement factors at 18.8 T of more than 100 in small molecules and globular proteins and also exhibits strong DNP enhancements in membrane proteins and cellular preparations. By integrating optimal sensitivity and high resolution, we expect widespread applications of this new polarizing agent in high-field DNP/ssNMR spectroscopy, especially for complex biomolecules.