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Article Dans Une Revue Angewandte Chemie International Edition Année : 2022

Highly efficient polarizing agents for MAS‐DNP of proton‐dense molecular solids

Thomas Halbritter
Fabien Aussenac
Krishna Damodaran
Daniel Lee
Sabine Hediger

Résumé

Efficiently hyperpolarizing proton-dense molecular solids through Dynamic Nuclear Polarization (DNP) solid-state NMR is still an unmet challenge. Polarizing agents (PAs) developed so far do not perform well on proton-rich systems, such as organic microcrystals and biomolecular assemblies. Herein we introduce a new PA, cAsymPol-POK, and report outstanding hyperpolarization efficiency on 12.76 kDa U-$^{13}$ C,$^{15}$ N-labeled LecA protein and pharmaceutical drugs at high magnetic fields (up to 18.8 T) and fast MAS frequencies (up to 40 kHz). The performance of cAsymPol-POK is rationalized by MAS-DNP simulations combined with Electron Paramagnetic Resonance (EPR), Density Functional Theory (DFT) and Molecular Dynamics (MD). This work shows that this new biradical is compatible with challenging biomolecular applications and unlocks the rapid acquisition of $^{13}$C-$^{13}$ C and $^{15}$N-$^{13}$C correlations of pharmaceutical drugs at natural isotopic abundance, which are key experiments for structure determination.
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Dates et versions

hal-03622904 , version 1 (07-04-2022)

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Rania Harrabi, Thomas Halbritter, Fabien Aussenac, Ons Dakhlaoui, Johan van Tol, et al.. Highly efficient polarizing agents for MAS‐DNP of proton‐dense molecular solids. Angewandte Chemie International Edition, 2022, 61 (12), pp.e202114103. ⟨10.1002/anie.202114103⟩. ⟨hal-03622904⟩
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