Reaction of OH radicals with CH3NH2 in the gas phase: Experimental (11.7-177.5 K) and computed rate coefficients (10-1000 K)

Nitrogen-bearing molecules, like methylamine (CH3NH2), can be the building blocks of amino acids in the interstellar medium (ISM). At the ultralow temperatures of the ISM, it is important to know its gas-phase reactivity towards interstellar radicals and the products formed. In this work, the kineti...

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Autores: González Fernández, Daniel, Lema Saavedra, Anxo, Espinosa, Sara, Martínez Núñez, Emilio, Fernández Ramos, Antonio, Canosa, André, Ballesteros Ruiz, Bernabé, Jiménez Martínez, Elena
Formato: artículo
Fecha de publicación:2022
País:España
Recursos:Universidad de Santiago de Compostela (USC)
Repositorio:Minerva. Repositorio Institucional de la Universidad de Santiago de Compostela
Idioma:inglés
OAI Identifier:oai:minerva.usc.gal:10347/45164
Acesso em linha:https://hdl.handle.net/10347/45164
Access Level:acceso abierto
Palavra-chave:OH radicals
Nitrogen-bearing molecules
Pressure regimes
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spelling Reaction of OH radicals with CH3NH2 in the gas phase: Experimental (11.7-177.5 K) and computed rate coefficients (10-1000 K)González Fernández, DanielLema Saavedra, AnxoEspinosa, SaraMartínez Núñez, EmilioFernández Ramos, AntonioCanosa, AndréBallesteros Ruiz, BernabéJiménez Martínez, ElenaOH radicalsNitrogen-bearing moleculesPressure regimesNitrogen-bearing molecules, like methylamine (CH3NH2), can be the building blocks of amino acids in the interstellar medium (ISM). At the ultralow temperatures of the ISM, it is important to know its gas-phase reactivity towards interstellar radicals and the products formed. In this work, the kinetics of the OH + CH3NH2 reaction was experimentally and theoretically investigated at low- and high-pressure limits (LPL and HPL) between 10 and 1000 K. Moreover, the CH2NH2 and CH3NH yields were computed in the same temperature range for both pressure regimes. A pulsed CRESU (French acronym for Reaction Kinetics in a Uniform Supersonic Flow) apparatus was employed to determine the rate coefficient, k(T), in the 11.7–177.5 K range. A drastic increase of k(T) when the temperature is lowered was observed in agreement with theoretical calculations, evaluated by the competitive canonical unified statistical (CCUS) theory, below 300 K in the LPL regime. The same trend was observed in the HPL regime below 350 K, but the theoretical k(T) values were higher than the experimental ones. Above 200 K, the calculated rate coefficients are improved with respect to previous computational studies and are in excellent agreement with the experimental literature data. In the LPL, the formation of CH3NH becomes largely dominant below ca. 100 K. Conversely, in the HPL regime, CH2NH2 is the only product below 100 K, whereas CH3NH becomes dominant at 298 K with a branching ratio similar to the one found in the LPL regime (≈70%). At T > 300 K, both reaction channels are competitive independently of the pressure regimeRoyal Society of ChemistryUniversidade de Santiago de Compostela. Centro de Investigación en Química Biolóxica e Materiais Moleculares (CiQUS)Universidade de Santiago de Compostela. Departamento de Química Física20222022-09-0620222022-09-06journal articlehttp://purl.org/coar/resource_type/c_6501AMhttp://purl.org/coar/version/c_ab4af688f83e57aainfo:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/10347/45164reponame:Minerva. Repositorio Institucional de la Universidad de Santiago de Compostelainstname:Universidad de Santiago de Compostela (USC)InglésengAgencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020 PID2020-113936GB-I00 QUIMICA INTERESTELAR RELEVANTE PARA EL ORIGEN DE LA VIDAAgencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020 PID2019-107307RB-I00 SIMULACION DE BIOCOMBUSTIBLES Y ADITIVOS DE GASOLINAopen accesshttp://purl.org/coar/access_right/c_abf2info:eu-repo/semantics/openAccessoai:minerva.usc.gal:10347/451642026-06-15T12:47:27Z
dc.title.none.fl_str_mv Reaction of OH radicals with CH3NH2 in the gas phase: Experimental (11.7-177.5 K) and computed rate coefficients (10-1000 K)
title Reaction of OH radicals with CH3NH2 in the gas phase: Experimental (11.7-177.5 K) and computed rate coefficients (10-1000 K)
spellingShingle Reaction of OH radicals with CH3NH2 in the gas phase: Experimental (11.7-177.5 K) and computed rate coefficients (10-1000 K)
González Fernández, Daniel
OH radicals
Nitrogen-bearing molecules
Pressure regimes
title_short Reaction of OH radicals with CH3NH2 in the gas phase: Experimental (11.7-177.5 K) and computed rate coefficients (10-1000 K)
title_full Reaction of OH radicals with CH3NH2 in the gas phase: Experimental (11.7-177.5 K) and computed rate coefficients (10-1000 K)
title_fullStr Reaction of OH radicals with CH3NH2 in the gas phase: Experimental (11.7-177.5 K) and computed rate coefficients (10-1000 K)
title_full_unstemmed Reaction of OH radicals with CH3NH2 in the gas phase: Experimental (11.7-177.5 K) and computed rate coefficients (10-1000 K)
title_sort Reaction of OH radicals with CH3NH2 in the gas phase: Experimental (11.7-177.5 K) and computed rate coefficients (10-1000 K)
dc.creator.none.fl_str_mv González Fernández, Daniel
Lema Saavedra, Anxo
Espinosa, Sara
Martínez Núñez, Emilio
Fernández Ramos, Antonio
Canosa, André
Ballesteros Ruiz, Bernabé
Jiménez Martínez, Elena
author González Fernández, Daniel
author_facet González Fernández, Daniel
Lema Saavedra, Anxo
Espinosa, Sara
Martínez Núñez, Emilio
Fernández Ramos, Antonio
Canosa, André
Ballesteros Ruiz, Bernabé
Jiménez Martínez, Elena
author_role author
author2 Lema Saavedra, Anxo
Espinosa, Sara
Martínez Núñez, Emilio
Fernández Ramos, Antonio
Canosa, André
Ballesteros Ruiz, Bernabé
Jiménez Martínez, Elena
author2_role author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Universidade de Santiago de Compostela. Centro de Investigación en Química Biolóxica e Materiais Moleculares (CiQUS)
Universidade de Santiago de Compostela. Departamento de Química Física
dc.subject.none.fl_str_mv OH radicals
Nitrogen-bearing molecules
Pressure regimes
topic OH radicals
Nitrogen-bearing molecules
Pressure regimes
description Nitrogen-bearing molecules, like methylamine (CH3NH2), can be the building blocks of amino acids in the interstellar medium (ISM). At the ultralow temperatures of the ISM, it is important to know its gas-phase reactivity towards interstellar radicals and the products formed. In this work, the kinetics of the OH + CH3NH2 reaction was experimentally and theoretically investigated at low- and high-pressure limits (LPL and HPL) between 10 and 1000 K. Moreover, the CH2NH2 and CH3NH yields were computed in the same temperature range for both pressure regimes. A pulsed CRESU (French acronym for Reaction Kinetics in a Uniform Supersonic Flow) apparatus was employed to determine the rate coefficient, k(T), in the 11.7–177.5 K range. A drastic increase of k(T) when the temperature is lowered was observed in agreement with theoretical calculations, evaluated by the competitive canonical unified statistical (CCUS) theory, below 300 K in the LPL regime. The same trend was observed in the HPL regime below 350 K, but the theoretical k(T) values were higher than the experimental ones. Above 200 K, the calculated rate coefficients are improved with respect to previous computational studies and are in excellent agreement with the experimental literature data. In the LPL, the formation of CH3NH becomes largely dominant below ca. 100 K. Conversely, in the HPL regime, CH2NH2 is the only product below 100 K, whereas CH3NH becomes dominant at 298 K with a branching ratio similar to the one found in the LPL regime (≈70%). At T > 300 K, both reaction channels are competitive independently of the pressure regime
publishDate 2022
dc.date.none.fl_str_mv 2022
2022-09-06
2022
2022-09-06
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
AM
http://purl.org/coar/version/c_ab4af688f83e57aa
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/10347/45164
url https://hdl.handle.net/10347/45164
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020 PID2020-113936GB-I00 QUIMICA INTERESTELAR RELEVANTE PARA EL ORIGEN DE LA VIDA
Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020 PID2019-107307RB-I00 SIMULACION DE BIOCOMBUSTIBLES Y ADITIVOS DE GASOLINA
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
dc.source.none.fl_str_mv reponame:Minerva. Repositorio Institucional de la Universidad de Santiago de Compostela
instname:Universidad de Santiago de Compostela (USC)
instname_str Universidad de Santiago de Compostela (USC)
reponame_str Minerva. Repositorio Institucional de la Universidad de Santiago de Compostela
collection Minerva. Repositorio Institucional de la Universidad de Santiago de Compostela
repository.name.fl_str_mv
repository.mail.fl_str_mv
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