Observing Nearby Nuclei on Paramagnetic Trityls and MOFs via DNP and Electron Decoupling.
dynamic nuclear polarization
electron decoupling
hyperpolarization
metal-organic framework
Journal
Chemistry (Weinheim an der Bergstrasse, Germany)
ISSN: 1521-3765
Titre abrégé: Chemistry
Pays: Germany
ID NLM: 9513783
Informations de publication
Date de publication:
06 Dec 2022
06 Dec 2022
Historique:
received:
17
08
2022
pubmed:
12
9
2022
medline:
15
12
2022
entrez:
11
9
2022
Statut:
ppublish
Résumé
Dynamic nuclear polarization (DNP) is an NMR sensitivity enhancement technique that mediates polarization transfer from unpaired electrons to NMR-active nuclei. Despite its success in elucidating important structural information on biological and inorganic materials, the detailed polarization-transfer pathway from the electrons to the nearby and then the bulk solvent nuclei, and finally to the molecules of interest-remains unclear. In particular, the nuclei in the paramagnetic polarizing agent play significant roles in relaying the enhanced NMR polarizations to more remote nuclei. Despite their importance, the direct NMR observation of these nuclei is challenging because of poor sensitivity. Here, we show that a combined DNP and electron decoupling approach can facilitate direct NMR detection of these nuclei. We achieved an ∼80 % improvement in NMR intensity via electron decoupling at 0.35 T and 80 K on trityl radicals. Moreover, we recorded a DNP enhancement factor of
Identifiants
pubmed: 36089532
doi: 10.1002/chem.202202556
pmc: PMC9795816
mid: NIHMS1859952
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
e202202556Subventions
Organisme : NIBIB NIH HHS
ID : R00 EB023990
Pays : United States
Organisme : Natural Science Foundation
ID : DMR-2105495
Organisme : Agence Nationale de la Recherche
ID : ANR-20-ERC9-0008
Organisme : NIBIB NIH HHS
ID : K99 EB023990
Pays : United States
Organisme : NIBIB NIH HHS
ID : EB023990
Pays : United States
Organisme : NIGMS NIH HHS
ID : GM132997
Pays : United States
Organisme : NIGMS NIH HHS
ID : GM132079
Pays : United States
Organisme : NIGMS NIH HHS
ID : R01 GM132997
Pays : United States
Organisme : NIGMS NIH HHS
ID : P41 GM132079
Pays : United States
Organisme : NIBIB NIH HHS
ID : EB028553
Pays : United States
Organisme : NIBIB NIH HHS
ID : R21 EB028553
Pays : United States
Informations de copyright
© 2022 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH.
Références
Prog Nucl Magn Reson Spectrosc. 2019 Apr;111:1-271
pubmed: 31146806
Chembiochem. 2005 Sep;6(9):1536-49
pubmed: 16094696
Prog Nucl Magn Reson Spectrosc. 2017 Nov;102-103:120-195
pubmed: 29157490
Phys Rev B Condens Matter. 1985 Nov 1;32(9):5608-5627
pubmed: 9937807
Sci Adv. 2019 Jan 18;5(1):eaav6909
pubmed: 30746482
J Chem Phys. 2017 Oct 28;147(16):164201
pubmed: 29096491
J Magn Reson. 2012 Jan;214(1):29-41
pubmed: 22119645
J Magn Reson. 2018 Apr;289:45-54
pubmed: 29471275
J Chem Phys. 2015 Aug 7;143(5):054201
pubmed: 26254646
Phys Chem Chem Phys. 2021 Jan 21;23(2):1006-1020
pubmed: 33404028
Bioorg Med Chem Lett. 2008 Aug 1;18(15):4291-3
pubmed: 18640034
Sci Adv. 2019 Jul 26;5(7):eaax2743
pubmed: 31360772
J Am Chem Soc. 2021 Dec 8;143(48):20281-20290
pubmed: 34813311
J Phys Chem Lett. 2016 Jan 7;7(1):111-6
pubmed: 26651876
Bioorg Med Chem Lett. 2010 Jul 1;20(13):3946-9
pubmed: 20537895
J Am Chem Soc. 2017 May 10;139(18):6310-6313
pubmed: 28429936
Chemistry. 2022 Dec 6;28(68):e202202556
pubmed: 36089532
Sci Adv. 2021 Apr 30;7(18):
pubmed: 33931450
J Chem Phys. 2013 Dec 7;139(21):214201
pubmed: 24320373
Angew Chem Int Ed Engl. 2014 Sep 1;53(36):9476-81
pubmed: 25044761
Angew Chem Int Ed Engl. 2019 May 27;58(22):7259-7262
pubmed: 30921488