Journal of the American Chemical Society, volume 139, issue 28, pages 9551-9557
Conformational Switching of HOCO Radical: Selective Vibrational Excitation and Hydrogen-Atom Tunneling
Publication type: Journal Article
Publication date: 2017-07-05
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor: 15
ISSN: 00027863, 15205126
General Chemistry
Catalysis
Biochemistry
Colloid and Surface Chemistry
Abstract
Conformers of carboxyl radical (HOCO) have been studied by IR spectroscopy in argon and nitrogen matrices. In an argon matrix, only the lower-energy conformer trans-HOCO is observed, whereas both cis and trans conformers are found for deuterated carboxyl radical DOCO. In a nitrogen matrix, both conformers of HOCO and DOCO isotopologues can be prepared, indicating strong stabilization of the higher-energy cis conformer by a nitrogen matrix. Selective vibrational excitation promotes the trans-to-cis and cis-to-trans conversions of DOCO in an argon matrix and HOCO and DOCO in a nitrogen matrix, which is the first conformational photoswitching of an open-shell species. In a nitrogen matrix, the cis-to-trans and trans-to-cis conversions of HOCO is also found upon broadband IR light of the spectrometer, and the ratio of the quantum yields of these processes is about 3.3. The photoswitching peculiarities are in agreement with the available theoretical energy barriers. The higher-energy cis conformer decays to the lower-energy trans conformer via hydrogen-atom tunneling through the torsional barrier, which is also a unique observation for an open-shell species. The tunneling mechanism of the cis-to-trans switching is supported by the low-temperature limit of the reaction rate and by the H/D kinetic isotope effect. Our results suggest a large difference in the H/D kinetic isotope effects in nitrogen and argon matrices (∼5 and >100, respectively). The stabilizing effect on cis-DOCO by a nitrogen matrix (by 2 orders of magnitude versus an argon matrix) is much smaller than that on cis-HOCO (estimated to be >104).
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Citations by publishers
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1 publication, 3.23%
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1 publication, 3.23%
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Springer Nature
1 publication, 3.23%
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- We do not take into account publications that without a DOI.
- Statistics recalculated only for publications connected to researchers, organizations and labs registered on the platform.
- Statistics recalculated weekly.
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Ryazantsev S. V. et al. Conformational Switching of HOCO Radical: Selective Vibrational Excitation and Hydrogen-Atom Tunneling // Journal of the American Chemical Society. 2017. Vol. 139. No. 28. pp. 9551-9557.
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Ryazantsev S. V., Feldman V. I., Khriachtchev L. Conformational Switching of HOCO Radical: Selective Vibrational Excitation and Hydrogen-Atom Tunneling // Journal of the American Chemical Society. 2017. Vol. 139. No. 28. pp. 9551-9557.
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TY - JOUR
DO - 10.1021/jacs.7b02605
UR - https://doi.org/10.1021%2Fjacs.7b02605
TI - Conformational Switching of HOCO Radical: Selective Vibrational Excitation and Hydrogen-Atom Tunneling
T2 - Journal of the American Chemical Society
AU - Ryazantsev, Sergey V
AU - Khriachtchev, Leonid
AU - Feldman, Vladimir I.
PY - 2017
DA - 2017/07/05 00:00:00
PB - American Chemical Society (ACS)
SP - 9551-9557
IS - 28
VL - 139
SN - 0002-7863
SN - 1520-5126
ER -
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@article{2017_Ryazantsev,
author = {Sergey V Ryazantsev and Leonid Khriachtchev and Vladimir I. Feldman},
title = {Conformational Switching of HOCO Radical: Selective Vibrational Excitation and Hydrogen-Atom Tunneling},
journal = {Journal of the American Chemical Society},
year = {2017},
volume = {139},
publisher = {American Chemical Society (ACS)},
month = {jul},
url = {https://doi.org/10.1021%2Fjacs.7b02605},
number = {28},
pages = {9551--9557},
doi = {10.1021/jacs.7b02605}
}
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Ryazantsev, Sergey V., et al. “Conformational Switching of HOCO Radical: Selective Vibrational Excitation and Hydrogen-Atom Tunneling.” Journal of the American Chemical Society, vol. 139, no. 28, Jul. 2017, pp. 9551-9557. https://doi.org/10.1021%2Fjacs.7b02605.