Journal of the American Chemical Society, volume 143, issue 21, pages 8164-8176
Platform for High-Spin Molecules: A Verdazyl-Nitronyl Nitroxide Triradical with Quartet Ground State
Tretyakov Evgeny
1
,
Petunin Pavel
2
,
Gorbunov Dmitry
4
,
Gritsan N.P
4
,
Fedin Matvey
5
,
Stass Dmitri V
4, 6
,
Samoilova Rimma I.
4
,
Shundrina Inna K.
3
,
Trusova Marina E
2
,
Publication type: Journal Article
Publication date: 2021-05-21
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor: 15
ISSN: 00027863, 15205126
General Chemistry
Catalysis
Biochemistry
Colloid and Surface Chemistry
Abstract
Thermally resistant air-stable organic triradicals with a quartet ground state and a large energy gap between spin states are still unique compounds. In this work, we succeeded to design and prepare the first highly stable triradical, consisting of oxoverdazyl and nitronyl nitroxide radical fragments, with a quartet ground state. The triradical and its diradical precursor were synthesized via a palladium-catalyzed cross-coupling reaction of diiodoverdazyl with nitronyl nitroxide-2-ide gold(I) complex. Both paramagnetic compounds were fully characterized by single-crystal X-ray diffraction analysis, superconducting quantum interference device magnetometry, EPR spectroscopy in various matrices, and cyclic voltammetry. In the diradical, the verdazyl and nitronyl nitroxide centers demonstrated full reversibility of redox process, while for the triradical, the electrochemical reduction and oxidation proceed at practically the same redox potentials, but become quasi-reversible. A series of high-level CASSCF/NEVPT2 calculations was performed to predict inter- and intramolecular exchange interactions in crystals of di- and triradicals and to establish their magnetic motifs. Based on the predicted magnetic motifs, the temperature dependences of the magnetic susceptibility were analyzed, and the singlet-triplet (135 ± 10 cm-1) and doublet-quartet (17 ± 2 and 152 ± 19 cm-1) splitting was found to be moderate. Unique high stability of synthesized verdazyl-nitronylnitroxide triradical opens new perspectives for further functionalization and design of high-spin systems with four or more spins.
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Tretyakov E. et al. Platform for High-Spin Molecules: A Verdazyl-Nitronyl Nitroxide Triradical with Quartet Ground State // Journal of the American Chemical Society. 2021. Vol. 143. No. 21. pp. 8164-8176.
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Tretyakov E., Petunin P., Zhivetyeva S., Gorbunov D., Gritsan N., Fedin M., Stass D. V., Samoilova R. I., Bagryanskaya I. Y., Shundrina I. K., Bogomyakov A. S., Kazantsev M. S., Postnikov P. S., Trusova M. E., Ovcharenko V. Platform for High-Spin Molecules: A Verdazyl-Nitronyl Nitroxide Triradical with Quartet Ground State // Journal of the American Chemical Society. 2021. Vol. 143. No. 21. pp. 8164-8176.
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TY - JOUR
DO - 10.1021/jacs.1c02938
UR - https://doi.org/10.1021%2Fjacs.1c02938
TI - Platform for High-Spin Molecules: A Verdazyl-Nitronyl Nitroxide Triradical with Quartet Ground State
T2 - Journal of the American Chemical Society
AU - Stass, Dmitri V
AU - Trusova, Marina E
AU - Petunin, Pavel
AU - Gritsan, N.P
AU - Fedin, Matvey
AU - Bogomyakov, Artem S
AU - Kazantsev, Maxim S.
AU - Postnikov, Pavel S.
AU - Tretyakov, Evgeny
AU - Zhivetyeva, Svetlana
AU - Gorbunov, Dmitry
AU - Samoilova, Rimma I.
AU - Bagryanskaya, Irina Yu.
AU - Shundrina, Inna K.
AU - Ovcharenko, V.
PY - 2021
DA - 2021/05/21 00:00:00
PB - American Chemical Society (ACS)
SP - 8164-8176
IS - 21
VL - 143
SN - 0002-7863
SN - 1520-5126
ER -
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@article{2021_Tretyakov,
author = {Dmitri V Stass and Marina E Trusova and Pavel Petunin and N.P Gritsan and Matvey Fedin and Artem S Bogomyakov and Maxim S. Kazantsev and Pavel S. Postnikov and Evgeny Tretyakov and Svetlana Zhivetyeva and Dmitry Gorbunov and Rimma I. Samoilova and Irina Yu. Bagryanskaya and Inna K. Shundrina and V. Ovcharenko},
title = {Platform for High-Spin Molecules: A Verdazyl-Nitronyl Nitroxide Triradical with Quartet Ground State},
journal = {Journal of the American Chemical Society},
year = {2021},
volume = {143},
publisher = {American Chemical Society (ACS)},
month = {may},
url = {https://doi.org/10.1021%2Fjacs.1c02938},
number = {21},
pages = {8164--8176},
doi = {10.1021/jacs.1c02938}
}
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Tretyakov, Evgeny, et al. “Platform for High-Spin Molecules: A Verdazyl-Nitronyl Nitroxide Triradical with Quartet Ground State.” Journal of the American Chemical Society, vol. 143, no. 21, May. 2021, pp. 8164-8176. https://doi.org/10.1021%2Fjacs.1c02938.