Highly Efficient Trityl-Nitroxide Biradicals for Biomolecular High-Field Dynamic Nuclear Polarization

被引：26

作者：

Cai, Xinyi ^{[1
]}

Paioni, Alessandra Lucini ^{[2
]}

Adler, Agnes ^{[2
]}

Yao, Ru ^{[1
]}

Zhang, Wenxiao ^{[1
]}

Beriashvili, David ^{[2
]}

Safeer, Adil ^{[2
]}

Gurinov, Andrei ^{[2
]}

Rockenbauer, Antal ^{[3
,4
]}

Song, Yuguang ^{[1
]}

Baldus, Marc ^{[2
]}

Liu, Yangping ^{[1
]}

机构：

[1] Tianjin Med Univ, Sch Pharm, Prov & Minist Cosponsored Collaborat Innovat Ctr, Tianjin Key Lab Technol Enabling Dev Clin Therape, Tianjin 300070, Peoples R China

[2] Univ Utrecht, Bijvoet Ctr Biomol Res, NMR Spect Grp, Padualaan 8, NL-3584 CH Utrecht, Netherlands

[3] Hungarian Acad Sci, Inst Mat & Environm Chem, Budafoki Ut 8, H-1111 Budapest, Hungary

[4] Budapest Univ Technol & Econ, Dept Phys, Budafoki Ut 8, H-1111 Budapest, Hungary

来源：

CHEMISTRY-A EUROPEAN JOURNAL | 2021年 / 27卷 / 50期

基金：

中国国家自然科学基金;

关键词：

biradicals; dynamic nuclear polarization; polarizing agents; electron paramagnetic resonance; solid-state NMR spectroscopy; ENHANCED NMR-SPECTROSCOPY; POLARIZING AGENTS; GLASSY SOLVENTS; MAS; RADICALS; PROTEINS;

D O I：

10.1002/chem.202102253

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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.

引用

页码：12758 / 12762

页数：5

共 51 条

[41] Open and Closed Radicals: Local Geometry around Unpaired Electrons Governs Magic-Angle Spinning Dynamic Nuclear Polarization Performance [J].

Stevanato, Gabriele ;

Casano, Gilles ;

Kubicki, Dominik J. ;

Rao, Yu ;

Hofer, Laura Esteban ;

Menzildjian, Georges ;

Karoui, Hakim ;

Siri, Didier ;

Cordova, Manuel ;

Yulikov, Maxim ;

Jeschke, Gunnar ;

Lelli, Moreno ;

Lesage, Anne ;

Ouari, Olivier ;

Emsley, Lyndon .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2020, 142 (39) :16587-16599

[42] Magic Angle Spinning NMR of Proteins: High-Frequency Dynamic Nuclear Polarization and 1H Detection [J].

Su, Yongchao ;

Andreas, Loren ;

Griffin, Robert G. .

ANNUAL REVIEW OF BIOCHEMISTRY, VOL 84, 2015, 84 :465-497

[43] Dynamic nuclear polarization for sensitivity enhancement in modern solid-state NMR [J].

Thankamony, Aany Sofia Lilly ;

Wittmann, Johannes J. ;

Kaushik, Monu ;

Corzilius, Bjoern .

PROGRESS IN NUCLEAR MAGNETIC RESONANCE SPECTROSCOPY, 2017, 102 :120-195

[44] Theory for cross effect dynamic nuclear polarization under magic-angle spinning in solid state nuclear magnetic resonance: The importance of level crossings [J].

Thurber, Kent R. ;

Tycko, Robert .

JOURNAL OF CHEMICAL PHYSICS, 2012, 137 (08)

[45] Intracellular delivery of liposome-encapsulated Finland trityl radicals for EPR oximetry [J].

Wang, Xing ;

Peng, Chao ;

He, Ke ;

Ji, Kaiyun ;

Tan, Xiaoli ;

Han, Guifang ;

Liu, Yanxia ;

Liu, Yangping ;

Song, Yuguang .

ANALYST, 2020, 145 (14) :4964-4971

[46] BDPA-Nitroxide Biradicals Tailored for Efficient Dynamic Nuclear Polarization Enhanced Solid-State NMR at Magnetic Fields up to 21.1 T [J].

Wisser, Dorothea ;

Karthikeyan, Ganesan ;

Lund, Alicia ;

Casano, Gilles ;

Karoui, Hakim ;

Yulikov, Maxim ;

Menzildjian, Georges ;

Pinon, Arthur C. ;

Purea, Armin ;

Engelke, Frank ;

Chaudhari, Sachin R. ;

Kubicki, Dominik ;

Rossini, Aaron J. ;

Moroz, Ilia B. ;

Gajan, David ;

Coperet, Christophe ;

Jeschke, Gunnar ;

Lelli, Moreno ;

Emsley, Lyndon ;

Lesage, Anne ;

Ouari, Olivier .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2018, 140 (41) :13340-13349

[47] Large Molecular Weight Nitroxide Biradicals Providing Efficient Dynamic Nuclear Polarization at Temperatures up to 200 K [J].

Zagdoun, Alexandre ;

Casano, Gilles ;

Ouari, Olivier ;

Schwaerzwalder, Martin ;

Rossini, Aaron J. ;

Aussenac, Fabien ;

Yulikov, Maxim ;

Jeschke, Gunnar ;

Coperet, Christophe ;

Lesage, Anne ;

Tordo, Paul ;

Emsley, Lyndon .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2013, 135 (34) :12790-12797

[48] A Slowly Relaxing Rigid Biradical for Efficient Dynamic Nuclear Polarization Surface-Enhanced NMR Spectroscopy: Expeditious Characterization of Functional Group Manipulation in Hybrid Materials [J].

Zagdoun, Alexandre ;

Casano, Gilles ;

Ouari, Olivier ;

Lapadula, Giuseppe ;

Rossini, Aaron J. ;

Lelli, Moreno ;

Baffert, Mathieu ;

Gajan, David ;

Veyre, Laurent ;

Maas, Werner E. ;

Rosay, Melanie ;

Weber, Ralph T. ;

Thieuleux, Chloe ;

Coperet, Christophe ;

Lesage, Anne ;

Tordo, Paul ;

Emsley, Lyndon .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (04) :2284-2291

[49]

Zecevic A, 1998, MOL PHYS, V95, P1255, DOI 10.1080/00268979809483256

[50] Postmodification via Thiol-Click Chemistry Yields Hydrophilic Trityl-Nitroxide Biradicals for Biomolecular High-Field Dynamic Nuclear Polarization [J].

Zhai, Weixiang ;

Paioni, Alessandra Lucini ;

Cai, Xinyi ;

Narasimhan, Siddarth ;

Medeiros-Silva, Joao ;

Zhang, Wenxiao ;

Rockenbauer, Antal ;

Weingarth, Markus ;

Song, Yuguang ;

Baldus, Marc ;

Liu, Yangping .

JOURNAL OF PHYSICAL CHEMISTRY B, 2020, 124 (41) :9047-9060

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