Highly Efficient Trityl-nitroxide Biradicals for Biomolecular High-field Dynamic Nuclear Polarization

Xinyi Cai; Alessandra Lucini Paioni; Agnes Adler; Ru Yao; Wenxiao Zhang; David Beriashvili; Adil Safeer; Andrei Gurinov; Antal Rockenbauer; Yuguang Song; Marc Baldus; Yangping Liu

doi:10.1002/chem.202102253

Highly Efficient Trityl-nitroxide Biradicals for Biomolecular High-field Dynamic Nuclear Polarization

Xinyi Cai, Alessandra Lucini Paioni, Agnes Adler, Ru Yao, Wenxiao Zhang, David Beriashvili, Adil Safeer, Andrei Gurinov, Antal Rockenbauer, Yuguang Song, Marc Baldus, Yangping Liu

Tianjin Medical University
Hungarian Academy of Sciences Research Centre for Natural Sciences Institute of Materials and Environmental Chemistry: Termeszettudomanyi Kutatokozpont Anyag- es Kornyezetkemiai Intezet

Research output: Contribution to journal › Article › Academic › peer-review

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.

Original language	English
Pages (from-to)	12758-12762
Number of pages	5
Journal	Chemistry-A European Journal
Volume	27
Issue number	50
Early online date	28 Jun 2021
DOIs	https://doi.org/10.1002/chem.202102253
Publication status	Published - 6 Sept 2021

Bibliographical note

Funding Information:
We thank Raymond Schellevis for preparing the BamA sample, Johan van der Zwan for technical support and Weixiang Zhai for discussion about synthesis of SNAPols. This work was funded in part by the National Natural Science Foundation of China (Nos. 21871210 and 21572161 to Y.P.L.; No. 31500684 to Y.G.S.), the Netherlands Organization for Scientific Research (NWO) (Nos. 700.26.121, 700.10.443 and 718.015.001 to M.B.), Science & Technology Projects of Tianjin (No. 20JCZDJC00050 to Y.P.L.) and Hefei National Laboratory for Physical Sciences at the Microscale (KF2020001).

Publisher Copyright:
© 2021 Wiley-VCH GmbH

Keywords

biradicals
dynamic nuclear polarization
electron paramagnetic resonance
polarizing agents
solid-state NMR spectroscopy

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10.1002/chem.202102253

Chemistry A European J - 2021 - Cai - Highly Efficient Trityl‐Nitroxide Biradicals for Biomolecular High‐Field DynamicFinal published version, 2.77 MBLicence: Taverne

Cite this

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title = "Highly Efficient Trityl-nitroxide Biradicals for Biomolecular High-field Dynamic Nuclear Polarization",

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.",

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author = "Xinyi Cai and Paioni, {Alessandra Lucini} and Agnes Adler and Ru Yao and Wenxiao Zhang and David Beriashvili and Adil Safeer and Andrei Gurinov and Antal Rockenbauer and Yuguang Song and Marc Baldus and Yangping Liu",

note = "Funding Information: We thank Raymond Schellevis for preparing the BamA sample, Johan van der Zwan for technical support and Weixiang Zhai for discussion about synthesis of SNAPols. This work was funded in part by the National Natural Science Foundation of China (Nos. 21871210 and 21572161 to Y.P.L.; No. 31500684 to Y.G.S.), the Netherlands Organization for Scientific Research (NWO) (Nos. 700.26.121, 700.10.443 and 718.015.001 to M.B.), Science & Technology Projects of Tianjin (No. 20JCZDJC00050 to Y.P.L.) and Hefei National Laboratory for Physical Sciences at the Microscale (KF2020001). Publisher Copyright: {\textcopyright} 2021 Wiley-VCH GmbH",

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AU - Yao, Ru

AU - Zhang, Wenxiao

AU - Beriashvili, David

AU - Safeer, Adil

AU - Gurinov, Andrei

AU - Rockenbauer, Antal

AU - Song, Yuguang

AU - Baldus, Marc

AU - Liu, Yangping

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Highly Efficient Trityl-nitroxide Biradicals for Biomolecular High-field Dynamic Nuclear Polarization

Abstract

Bibliographical note

Keywords

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