scholarly journals Porous functionalized polymers enable generating and transporting hyperpolarized mixtures of metabolites

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Théo El Daraï ◽  
Samuel F. Cousin ◽  
Quentin Stern ◽  
Morgan Ceillier ◽  
James Kempf ◽  
...  
Keyword(s):  
Solid State ◽  
Dynamic Nuclear Polarization ◽  
Nuclear Polarization ◽  
Spin Diffusion ◽  
Relaxation Times ◽  
Functionalized Polymers ◽  
Cross Polarization ◽  
Biological Interest ◽  
Remote Preparation ◽  
Bulk Matrix

AbstractHyperpolarization by dissolution dynamic nuclear polarization (dDNP) has enabled promising applications in spectroscopy and imaging, but remains poorly widespread due to experimental complexity. Broad democratization of dDNP could be realized by remote preparation and distribution of hyperpolarized samples from dedicated facilities. Here we show the synthesis of hyperpolarizing polymers (HYPOPs) that can generate radical- and contaminant-free hyperpolarized samples within minutes with lifetimes exceeding hours in the solid state. HYPOPs feature tunable macroporous porosity, with porous volumes up to 80% and concentration of nitroxide radicals grafted in the bulk matrix up to 285 μmol g−1. Analytes can be efficiently impregnated as aqueous/alcoholic solutions and hyperpolarized up to P(13C) = 25% within 8 min, through the combination of 1H spin diffusion and 1H → 13C cross polarization. Solutions of 13C-analytes of biological interest hyperpolarized in HYPOPs display a very long solid-state 13C relaxation times of 5.7 h at 3.8 K, thus prefiguring transportation over long distances.

scholarly journals Revealing the Surface Structure of CdSe Nanocrystals by Dynamic Nuclear Polarization-Enhanced 77Se and 113Cd Solid-State NMR Spectroscopy

2021 ◽  
Author(s):  
Yunhua Chen ◽  
Rick Dorn ◽  
Michael Hanrahan ◽  
Lin Wei ◽  
Rafael Blome-Fernandez ◽  
...  
Keyword(s):  
Solid State ◽  
Dynamic Nuclear Polarization ◽  
Solid State Nmr ◽  
Nuclear Polarization ◽  
Surface Structures ◽  
Cdse Nanocrystals ◽  
Magic Angle ◽  
Cross Polarization ◽  
Zinc Blende ◽  
Detailed Surface

<p>Dynamic nuclear polarization (DNP) solid-state NMR (SSNMR) spectroscopy was used to obtain detailed surface structures of zinc blende CdSe nanocrystals (NCs) with plate or spheroidal morphologies and which are capped by carboxylic acid ligands. 1D <sup>113</sup>Cd and <sup>77</sup>Se cross-polarization magic angle spinning (CPMAS) NMR spectra revealed distinct signals from Cd and Se atoms on the surface of the NCs, and those residing in bulk-like environments below the surface. <sup>113</sup>Cd cross-polarization magic-angle-turning (CP-MAT) experiments identified CdSe<sub>3</sub>O, CdSe<sub>2</sub>O<sub>2</sub>, and CdSeO<sub>3</sub> Cd coordination environments on the surface of the NCs, where the oxygen atoms are presumably from coordinated carboxylate ligands. The sensitivity gain from DNP enabled natural isotopic abundance 2D homonuclear <sup>113</sup>Cd-<sup>113</sup>Cd and <sup>77</sup>Se-<sup>77</sup>Se and heteronuclear <sup>113</sup>Cd-<sup>77</sup>Se scalar correlation solid-state NMR experiments that reveal the connectivity of the Cd and Se atoms. Importantly, <sup>77</sup>Se{<sup>113</sup>Cd} scalar heteronuclear multiple quantum coherence (<i>J</i>-HMQC) experiments were used to selectively measure one-bond <sup>77</sup>Se-<sup>113</sup>Cd scalar coupling constants (<sup>1</sup><i>J</i>(<sup>77</sup>Se, <sup>113</sup>Cd)). With knowledge of <sup>1</sup><i>J</i>(<sup>77</sup>Se, <sup>113</sup>Cd), heteronuclear <sup>77</sup>Se{<sup>113</sup>Cd} spin echo (<i>J</i>-resolved) NMR experiments were then used to determine the number of Cd atoms bonded to Se atoms and vice versa. The <i>J</i>-resolved experiments directly confirmed that major Cd and Se surface species have CdSe<sub>2</sub>O<sub>2</sub> and SeCd<sub>4</sub> stoichiometries, respectively. Considering the crystal structure of zinc blende CdSe, and the similarity of the solid-state NMR data for the platelets and spheroids, we conclude that the surface of the spheroidal CdSe NCs is primarily composed of {100} facets. The methods outlined here will generally be applicable to obtain detailed surface structures of various main group semiconductors.</p>

scholarly journals Revealing the Surface Structure of CdSe Nanocrystals by Dynamic Nuclear Polarization-Enhanced 77Se and 113Cd Solid-State NMR Spectroscopy

2021 ◽  
Author(s):  
Yunhua Chen ◽  
Rick Dorn ◽  
Michael Hanrahan ◽  
Lin Wei ◽  
Rafael Blome-Fernandez ◽  
...  
Keyword(s):  
Solid State ◽  
Dynamic Nuclear Polarization ◽  
Solid State Nmr ◽  
Nuclear Polarization ◽  
Surface Structures ◽  
Cdse Nanocrystals ◽  
Magic Angle ◽  
Cross Polarization ◽  
Zinc Blende ◽  
Detailed Surface

<p>Dynamic nuclear polarization (DNP) solid-state NMR (SSNMR) spectroscopy was used to obtain detailed surface structures of zinc blende CdSe nanocrystals (NCs) with plate or spheroidal morphologies and which are capped by carboxylic acid ligands. 1D <sup>113</sup>Cd and <sup>77</sup>Se cross-polarization magic angle spinning (CPMAS) NMR spectra revealed distinct signals from Cd and Se atoms on the surface of the NCs, and those residing in bulk-like environments below the surface. <sup>113</sup>Cd cross-polarization magic-angle-turning (CP-MAT) experiments identified CdSe<sub>3</sub>O, CdSe<sub>2</sub>O<sub>2</sub>, and CdSeO<sub>3</sub> Cd coordination environments on the surface of the NCs, where the oxygen atoms are presumably from coordinated carboxylate ligands. The sensitivity gain from DNP enabled natural isotopic abundance 2D homonuclear <sup>113</sup>Cd-<sup>113</sup>Cd and <sup>77</sup>Se-<sup>77</sup>Se and heteronuclear <sup>113</sup>Cd-<sup>77</sup>Se scalar correlation solid-state NMR experiments that reveal the connectivity of the Cd and Se atoms. Importantly, <sup>77</sup>Se{<sup>113</sup>Cd} scalar heteronuclear multiple quantum coherence (<i>J</i>-HMQC) experiments were used to selectively measure one-bond <sup>77</sup>Se-<sup>113</sup>Cd scalar coupling constants (<sup>1</sup><i>J</i>(<sup>77</sup>Se, <sup>113</sup>Cd)). With knowledge of <sup>1</sup><i>J</i>(<sup>77</sup>Se, <sup>113</sup>Cd), heteronuclear <sup>77</sup>Se{<sup>113</sup>Cd} spin echo (<i>J</i>-resolved) NMR experiments were then used to determine the number of Cd atoms bonded to Se atoms and vice versa. The <i>J</i>-resolved experiments directly confirmed that major Cd and Se surface species have CdSe<sub>2</sub>O<sub>2</sub> and SeCd<sub>4</sub> stoichiometries, respectively. Considering the crystal structure of zinc blende CdSe, and the similarity of the solid-state NMR data for the platelets and spheroids, we conclude that the surface of the spheroidal CdSe NCs is primarily composed of {100} facets. The methods outlined here will generally be applicable to obtain detailed surface structures of various main group semiconductors.</p>

scholarly journals Dynamic Nuclear Polarization / solid-state NMR of membranes. Thermal effects and sample geometry

2019 ◽  
Vol 100 ◽  
pp. 70-76 ◽  
Author(s):  
Evgeniy Sergeevich Salnikov ◽  
Fabien Aussenac ◽  
Sebastian Abel ◽  
Armin Purea ◽  
Paul Tordo ◽  
...  
Keyword(s):  
Solid State ◽  
Dynamic Nuclear Polarization ◽  
Thermal Effects ◽  
Solid State Nmr ◽  
Nuclear Polarization ◽  
Sample Geometry

On The Potential of Dynamic Nuclear Polarization Enhanced Diamonds in Solid-State and Dissolution13C NMR Spectroscopy

ChemPhysChem ◽  
2016 ◽  
Vol 17 (17) ◽  
pp. 2691-2701 ◽  
Author(s):  
Christian O. Bretschneider ◽  
Ümit Akbey ◽  
Fabien Aussenac ◽  
Greg L. Olsen ◽  
Akiva Feintuch ◽  
...  
Keyword(s):  
Solid State ◽  
Nmr Spectroscopy ◽  
Dynamic Nuclear Polarization ◽  
Nuclear Polarization

scholarly journals Solid-State NMR/Dynamic Nuclear Polarization of Polypeptides in Planar Supported Lipid Bilayers

2015 ◽  
Vol 119 (46) ◽  
pp. 14574-14583 ◽  
Author(s):  
Evgeniy S. Salnikov ◽  
Hiba Sarrouj ◽  
Christian Reiter ◽  
Christopher Aisenbrey ◽  
Armin Purea ◽  
...  
Keyword(s):  
Solid State ◽  
Lipid Bilayers ◽  
Dynamic Nuclear Polarization ◽  
Solid State Nmr ◽  
Nuclear Polarization ◽  
Supported Lipid Bilayers

scholarly journals Solid-state NMR enhanced by dynamic nuclear polarization as a novel tool for ribosome structural biology

2013 ◽  
Vol 56 (2) ◽  
pp. 85-93 ◽  
Author(s):  
Ioannis Gelis ◽  
Veronika Vitzthum ◽  
Neha Dhimole ◽  
Marc A. Caporini ◽  
Andreas Schedlbauer ◽  
...  
Keyword(s):  
Solid State ◽  
Structural Biology ◽  
Dynamic Nuclear Polarization ◽  
Solid State Nmr ◽  
Nuclear Polarization

Up to 100% Improvement in Dynamic Nuclear Polarization Solid-State NMR Sensitivity Enhancement of Polymers by Removing Oxygen

2015 ◽  
Vol 36 (15) ◽  
pp. 1416-1421 ◽  
Author(s):  
Dao Le ◽  
Fabio Ziarelli ◽  
Trang N. T. Phan ◽  
Giulia Mollica ◽  
Pierre Thureau ◽  
...  
Keyword(s):  
Solid State ◽  
Dynamic Nuclear Polarization ◽  
Solid State Nmr ◽  
Nuclear Polarization ◽  
Sensitivity Enhancement ◽  
Nmr Sensitivity
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