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Theoretical kinetic study of the reactions between pyridyl radicals and O2

Konnov, Alexander A. LU ; Savchenkova, Anna S. ; Xie, Jibiao LU ; Matveev, Sergey S. ; Matveev, Sergey G. and Mebel, Alexander M. (2026) In Fuel 405.
Abstract

Reactions of the primary pyridine radicals, ortho-, meta-, and para-pyridyls with oxygen control the overall rate of pyridine oxidation. In the present work, the potential energy surfaces of o-, m-, and p-pyridyls + O2 previously developed by the authors have been employed for a systematic theoretical kinetic study of the rate constants of these reactions. The geometries of reactants, products, intermediates, and transition states of the reactions of pyridyl radicals with O2 were optimized at the level of density functional theory using the ωB97XD functional with the 6-311G** basis set. The temperature- and pressure-dependent rate constants of 31 reactions were evaluated within the framework of the... (More)

Reactions of the primary pyridine radicals, ortho-, meta-, and para-pyridyls with oxygen control the overall rate of pyridine oxidation. In the present work, the potential energy surfaces of o-, m-, and p-pyridyls + O2 previously developed by the authors have been employed for a systematic theoretical kinetic study of the rate constants of these reactions. The geometries of reactants, products, intermediates, and transition states of the reactions of pyridyl radicals with O2 were optimized at the level of density functional theory using the ωB97XD functional with the 6-311G** basis set. The temperature- and pressure-dependent rate constants of 31 reactions were evaluated within the framework of the Rice-Ramsperger-Kassel-Marcus (RRKM) theory combined with the Master Equation approach (RRKM–ME) in the temperature range from 300 to 3000 K, covering pressures from 0.01 to 100 atm. For several reactions previously investigated in the literature, good agreement was demonstrated, indicating consistency and correctness of the present theoretical calculations. Moreover, thermodynamic data for all important reactants, products, and intermediates have been revisited and calculated at the G4 theoretical level. The calculated rate constants and thermodynamic data provide a backbone for the development of detailed kinetic models for pyridine combustion.

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author
; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Oxidation, Pyridine, Pyridyl radicals, Rate constant, Thermodynamic data
in
Fuel
volume
405
article number
136713
publisher
Elsevier
external identifiers
  • scopus:105015034495
ISSN
0016-2361
DOI
10.1016/j.fuel.2025.136713
language
English
LU publication?
yes
id
df5ca0dd-dd40-48b6-a2ff-062a6d5115d6
date added to LUP
2025-10-01 16:09:30
date last changed
2025-10-14 09:57:29
@article{df5ca0dd-dd40-48b6-a2ff-062a6d5115d6,
  abstract     = {{<p>Reactions of the primary pyridine radicals, ortho-, meta-, and para-pyridyls with oxygen control the overall rate of pyridine oxidation. In the present work, the potential energy surfaces of o-, m-, and p-pyridyls + O<sub>2</sub> previously developed by the authors have been employed for a systematic theoretical kinetic study of the rate constants of these reactions. The geometries of reactants, products, intermediates, and transition states of the reactions of pyridyl radicals with O<sub>2</sub> were optimized at the level of density functional theory using the ωB97XD functional with the 6-311G** basis set. The temperature- and pressure-dependent rate constants of 31 reactions were evaluated within the framework of the Rice-Ramsperger-Kassel-Marcus (RRKM) theory combined with the Master Equation approach (RRKM–ME) in the temperature range from 300 to 3000 K, covering pressures from 0.01 to 100 atm. For several reactions previously investigated in the literature, good agreement was demonstrated, indicating consistency and correctness of the present theoretical calculations. Moreover, thermodynamic data for all important reactants, products, and intermediates have been revisited and calculated at the G4 theoretical level. The calculated rate constants and thermodynamic data provide a backbone for the development of detailed kinetic models for pyridine combustion.</p>}},
  author       = {{Konnov, Alexander A. and Savchenkova, Anna S. and Xie, Jibiao and Matveev, Sergey S. and Matveev, Sergey G. and Mebel, Alexander M.}},
  issn         = {{0016-2361}},
  keywords     = {{Oxidation; Pyridine; Pyridyl radicals; Rate constant; Thermodynamic data}},
  language     = {{eng}},
  month        = {{02}},
  publisher    = {{Elsevier}},
  series       = {{Fuel}},
  title        = {{Theoretical kinetic study of the reactions between pyridyl radicals and O<sub>2</sub>}},
  url          = {{http://dx.doi.org/10.1016/j.fuel.2025.136713}},
  doi          = {{10.1016/j.fuel.2025.136713}},
  volume       = {{405}},
  year         = {{2026}},
}