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Highly Efficient Trityl-Nitroxide Biradicals for Biomolecular High-Field Dynamic Nuclear Polarization |
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| Authors: | Xinyi Cai Dr Alessandra Lucini Paioni Agnes Adler Ru Yao Wenxiao Zhang David Beriashvili Adil Safeer Andrei Gurinov Prof Antal Rockenbauer Prof?Dr Yuguang Song Prof?Dr Marc Baldus Prof?Dr Yangping Liu |
| Institution: | 1. The province and ministry co-sponsored collaborative innovation center for medical epigenetics Tianjin Key Laboratory on Technologies Enabling Development of Clinical Therapeutics and Diagnostics School of Pharmacy, Tianjin Medical University, Tianjin, 300070 P. R. China
These authors contributed equally to this work.;2. NMR Spectroscopy group Bijvoet Center for Biomolecular Research, Utrecht University, Padualaan 8, 3584 CH Utrecht The Netherlands These authors contributed equally to this work.;3. NMR Spectroscopy group Bijvoet Center for Biomolecular Research, Utrecht University, Padualaan 8, 3584 CH Utrecht The Netherlands;4. The province and ministry co-sponsored collaborative innovation center for medical epigenetics Tianjin Key Laboratory on Technologies Enabling Development of Clinical Therapeutics and Diagnostics School of Pharmacy, Tianjin Medical University, Tianjin, 300070 P. R. China;5. Institute of Materials and Environmental Chemistry Hungarian Academy of Sciences and Department of Physics, Budapest University of Technology and Economics Budafoki ut 8, 1111 Budapest, Hungary |
| Abstract: | 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. |
| Keywords: | biradicals dynamic nuclear polarization polarizing agents electron paramagnetic resonance solid-state NMR spectroscopy |