Reactions of sulphate radicals with substituted pyridines: a structure–reactivity correlation analysis

The kinetics of the oxidation of pyridine, 3-chloropyridine, 3-cyanopyridine, 3-methoxypyridine and 3-methylpyridine mediated by SO₄<M>; radicals are studied by flash photolysis of peroxodisulphate, S₂O₈²⁻−, at pH 2.5 and 9. The absolute rate constants for the reactions of both, the basic and...

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Autores principales: Dell'Arciprete, María Laura, Cobos, Carlos Jorge, Furlong, Jorge Javier Pedro, Mártire, Daniel Osvaldo, González, Mónica Cristina
Formato: Articulo
Lenguaje:Inglés
Publicado: 2007
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Acceso en línea:http://sedici.unlp.edu.ar/handle/10915/159380
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spelling I19-R120-10915-1593802023-10-27T04:06:40Z http://sedici.unlp.edu.ar/handle/10915/159380 Reactions of sulphate radicals with substituted pyridines: a structure–reactivity correlation analysis Dell'Arciprete, María Laura Cobos, Carlos Jorge Furlong, Jorge Javier Pedro Mártire, Daniel Osvaldo González, Mónica Cristina 2007 2023-10-26T12:24:16Z en Química kinetics oxidation pyridine flash photolysis The kinetics of the oxidation of pyridine, 3-chloropyridine, 3-cyanopyridine, 3-methoxypyridine and 3-methylpyridine mediated by SO₄<M>; radicals are studied by flash photolysis of peroxodisulphate, S₂O₈²⁻−, at pH 2.5 and 9. The absolute rate constants for the reactions of both, the basic and acid forms of the pyridines, are determined and discussed in terms of the Hammett correlation. The monosubstituted pyridines react about 10 times faster with sulphate radicals than their protonated forms, the pyridine ions. The organic intermediates are identified as the corresponding hydroxypyridine radical adducts and their absorption spectra compared with those estimated employing the time-dependent density functional theory with explicit account for bulk solvent effects. A reaction mechanism which accounts for the observed intermediates and the pyridinols formed as products is proposed. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas Laboratorio de Estudio de Compuestos Orgánicos Articulo Articulo http://creativecommons.org/licenses/by-nc-sa/4.0/ Creative Commons Attribution-NonCommercial-ShareAlike 4.0 International (CC BY-NC-SA 4.0) application/pdf 2498-2505
institution Universidad Nacional de La Plata
institution_str I-19
repository_str R-120
collection SEDICI (UNLP)
language Inglés
topic Química
kinetics
oxidation
pyridine
flash photolysis
spellingShingle Química
kinetics
oxidation
pyridine
flash photolysis
Dell'Arciprete, María Laura
Cobos, Carlos Jorge
Furlong, Jorge Javier Pedro
Mártire, Daniel Osvaldo
González, Mónica Cristina
Reactions of sulphate radicals with substituted pyridines: a structure–reactivity correlation analysis
topic_facet Química
kinetics
oxidation
pyridine
flash photolysis
description The kinetics of the oxidation of pyridine, 3-chloropyridine, 3-cyanopyridine, 3-methoxypyridine and 3-methylpyridine mediated by SO₄<M>; radicals are studied by flash photolysis of peroxodisulphate, S₂O₈²⁻−, at pH 2.5 and 9. The absolute rate constants for the reactions of both, the basic and acid forms of the pyridines, are determined and discussed in terms of the Hammett correlation. The monosubstituted pyridines react about 10 times faster with sulphate radicals than their protonated forms, the pyridine ions. The organic intermediates are identified as the corresponding hydroxypyridine radical adducts and their absorption spectra compared with those estimated employing the time-dependent density functional theory with explicit account for bulk solvent effects. A reaction mechanism which accounts for the observed intermediates and the pyridinols formed as products is proposed.
format Articulo
Articulo
author Dell'Arciprete, María Laura
Cobos, Carlos Jorge
Furlong, Jorge Javier Pedro
Mártire, Daniel Osvaldo
González, Mónica Cristina
author_facet Dell'Arciprete, María Laura
Cobos, Carlos Jorge
Furlong, Jorge Javier Pedro
Mártire, Daniel Osvaldo
González, Mónica Cristina
author_sort Dell'Arciprete, María Laura
title Reactions of sulphate radicals with substituted pyridines: a structure–reactivity correlation analysis
title_short Reactions of sulphate radicals with substituted pyridines: a structure–reactivity correlation analysis
title_full Reactions of sulphate radicals with substituted pyridines: a structure–reactivity correlation analysis
title_fullStr Reactions of sulphate radicals with substituted pyridines: a structure–reactivity correlation analysis
title_full_unstemmed Reactions of sulphate radicals with substituted pyridines: a structure–reactivity correlation analysis
title_sort reactions of sulphate radicals with substituted pyridines: a structure–reactivity correlation analysis
publishDate 2007
url http://sedici.unlp.edu.ar/handle/10915/159380
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AT coboscarlosjorge reactionsofsulphateradicalswithsubstitutedpyridinesastructurereactivitycorrelationanalysis
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AT martiredanielosvaldo reactionsofsulphateradicalswithsubstitutedpyridinesastructurereactivitycorrelationanalysis
AT gonzalezmonicacristina reactionsofsulphateradicalswithsubstitutedpyridinesastructurereactivitycorrelationanalysis
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