at Google ScholarTitle data
van der Zwan, Kasper P. ; Riedel, Wiebke ; Aussenac, Fabien ; Reiter, Christian ; Kreger, Klaus ; Schmidt, Hans-Werner ; Risse, Thomas ; Gutmann, Torsten ; Senker, Jürgen:
F-19 MAS DNP for Probing Molecules in Nanomolar Concentrations : Direct Polarization as Key for Solid-State NMR Spectra without Solvent and Matrix Signals.
In: The Journal of Physical Chemistry C.
Vol. 125
(2021)
Issue 13
.
- pp. 7287-7296.
ISSN 1932-7455
DOI: https://doi.org/10.1021/acs.jpcc.1c01167
Abstract in another language
The efficiency of dynamic nuclear polarization (DNP) enhanced F-19 MAS NMR spectroscopy without F-19-containing solvents and matrices, which transport polarization via F-19-F-19 spin diffusion, is demonstrated. By preventing solvent and matrix signals respectively masking the corresponding resonances, this enables the detection of fluorinated target molecules in nanomolar amounts. As model compound, 1,3,5-tris(2-fluoro-2-methylpropionylamino)benzene (F-BTA) is investigated in a frozen 1,1,2,2-tetrachloroethane (TCE) solution and incorporated into a matrix of isotactic polypropylene (i-PP). While the polarizing agent is homogeneously dissolved within the frozen solution, for the i-PP/F-BTA blend, it is distributed via the incipient wetness impregnation (IWI) technique. For the frozen solutions with an F-BTA concentration of 187.5 mM an epsilon(on/off) of 260 was obtained. For F-BTA concentrations of 10 and 2.5 mM the sensitivity trend suggests even higher DNP gains. The substantial enhancements could be achieved by direct polarization transfer over distances up to at least 20 A, derived from a simple geometric model assuming a homogeneous solution, engaging a large part of the sample volume. Cross-polarization (CP) to C-13 nuclei allowed selection of the NMR spectroscopic resonances of the minority species in the i-PP/F-BTA blend suppressing the otherwise dominating resonances of the IWI solvent and the polymer matrix. The possibility of exciting F-19 via DNP directly and of transferring the polarization to other heteronuclei within close proximity enables spatial spectral editing to clear up spectra otherwise crowded by matrix and solvent signals. We thus expect direct polarization transfer techniques for DNP enhanced NMR spectroscopy to become more important in the future.
Further data
| Item Type: | Article in a journal |
|---|---|
| Refereed: | Yes |
| Additional notes: | ISI:000639044400027 |
| Institutions of the University: | Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Chair Inorganic Chemistry III > Chair Inorganic Chemistry III - Univ.-Prof. Dr. Jürgen Senker Research Institutions > Research Centres > Nordbayerisches Zentrum für NMR-Spektroskopie - NMR-Zentrum Faculties Faculties > Faculty of Biology, Chemistry and Earth Sciences Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Chair Inorganic Chemistry III Research Institutions Research Institutions > Research Centres |
| Result of work at the UBT: | Yes |
| DDC Subjects: | 500 Science 500 Science > 540 Chemistry |
| Date Deposited: | 08 Jun 2021 08:00 |
| Last Modified: | 05 Apr 2023 06:05 |
| URI: | https://eref.uni-bayreuth.de/id/eprint/65687 |