A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation

Autores
Hossaini, Ryan; Chipperfield, Martyn P.; Saiz Lopez, Alfonso; Fernandez, Rafael Pedro; Monks, Sarah; Feng, Wuhu; Brauer, Peter; Von Glasow, Roland
Año de publicación
2016
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Chlorine atoms (Cl) are highly reactive toward hydrocarbons in the Earth’s troposphere, including the greenhouse gas methane (CH4). However, the regional and global CH4 sink from Cl is poorly quantified as tropospheric Cl concentrations ([Cl]) are uncertain by ~2 orders of magnitude. Here we describe the addition of a detailed tropospheric chlorine scheme to the TOMCAT chemical transport model. The model includes several sources of tropospheric inorganic chlorine (Cly), including (i) the oxidation of chlorocarbons of natural (CH3Cl, CHBr2Cl, CH2BrCl, and CHBrCl2) and anthropogenic (CH2Cl2, CHCl3, C2Cl4, C2HCl3, and CH2ClCH2Cl) origin and (ii) sea-salt aerosol dechlorination. Simulations were performed to quantify tropospheric [Cl], with a focus on the marine boundary layer, and quantify the global significance of Cl atom CH4 oxidation. In agreement with observations, simulated surface levels of hydrogen chloride (HCl), the most abundant Cly reservoir, reach several parts per billion (ppb) over polluted coastal/continental regions, with sub-ppb levels typical in more remote regions. Modeled annual mean surface [Cl] exhibits large spatial variability with the largest levels, typically in the range of 1-5×104 atoms cm-3, in the polluted northern hemisphere. Chlorocarbon oxidation provides a tropospheric Cly source of up to ~4320 Gg Cl/yr, sustaining a background surface [Cl] of <0.1 to 0.5 × 103 atoms cm-3 over large areas. Globally, we estimate a tropospheric methane sink of ~12-13 Tg CH4/yr due the CH4 + Cl reaction (~2.5% of total CH4 oxidation). Larger regional effects are predicted, with Cl accounting for ~10 to >20% of total boundary layer CH4 oxidation in some locations.
Fil: Hossaini, Ryan. University of Lancaster; Reino Unido
Fil: Chipperfield, Martyn P.. University of Leeds; Reino Unido
Fil: Saiz Lopez, Alfonso. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; España
Fil: Fernandez, Rafael Pedro. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; España. Universidad Tecnologica Nacional. Facultad Regional Mendoza. Secretaría de Ciencia, Tecnología y Postgrado; Argentina. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina
Fil: Monks, Sarah. National Center For Atmospheric Research. Amospheric Chemistry División; Estados Unidos. University of Colorado Boulder; Estados Unidos
Fil: Feng, Wuhu. University of Leeds; Reino Unido
Fil: Brauer, Peter. University of New York; Estados Unidos. University of East Anglia; Reino Unido
Fil: Von Glasow, Roland. University of East Anglia; Reino Unido
Materia
TROPOSPHERIC CHLORINE
METHANE OXIDATION
VSL CHEMISTRY
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/100772
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/100772
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidationHossaini, RyanChipperfield, Martyn P.Saiz Lopez, AlfonsoFernandez, Rafael PedroMonks, SarahFeng, WuhuBrauer, PeterVon Glasow, RolandTROPOSPHERIC CHLORINEMETHANE OXIDATIONVSL CHEMISTRYhttps://purl.org/becyt/ford/1.5https://purl.org/becyt/ford/1Chlorine atoms (Cl) are highly reactive toward hydrocarbons in the Earth’s troposphere, including the greenhouse gas methane (CH4). However, the regional and global CH4 sink from Cl is poorly quantified as tropospheric Cl concentrations ([Cl]) are uncertain by ~2 orders of magnitude. Here we describe the addition of a detailed tropospheric chlorine scheme to the TOMCAT chemical transport model. The model includes several sources of tropospheric inorganic chlorine (Cly), including (i) the oxidation of chlorocarbons of natural (CH3Cl, CHBr2Cl, CH2BrCl, and CHBrCl2) and anthropogenic (CH2Cl2, CHCl3, C2Cl4, C2HCl3, and CH2ClCH2Cl) origin and (ii) sea-salt aerosol dechlorination. Simulations were performed to quantify tropospheric [Cl], with a focus on the marine boundary layer, and quantify the global significance of Cl atom CH4 oxidation. In agreement with observations, simulated surface levels of hydrogen chloride (HCl), the most abundant Cly reservoir, reach several parts per billion (ppb) over polluted coastal/continental regions, with sub-ppb levels typical in more remote regions. Modeled annual mean surface [Cl] exhibits large spatial variability with the largest levels, typically in the range of 1-5×104 atoms cm-3, in the polluted northern hemisphere. Chlorocarbon oxidation provides a tropospheric Cly source of up to ~4320 Gg Cl/yr, sustaining a background surface [Cl] of <0.1 to 0.5 × 103 atoms cm-3 over large areas. Globally, we estimate a tropospheric methane sink of ~12-13 Tg CH4/yr due the CH4 + Cl reaction (~2.5% of total CH4 oxidation). Larger regional effects are predicted, with Cl accounting for ~10 to >20% of total boundary layer CH4 oxidation in some locations.Fil: Hossaini, Ryan. University of Lancaster; Reino UnidoFil: Chipperfield, Martyn P.. University of Leeds; Reino UnidoFil: Saiz Lopez, Alfonso. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; EspañaFil: Fernandez, Rafael Pedro. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; España. Universidad Tecnologica Nacional. Facultad Regional Mendoza. Secretaría de Ciencia, Tecnología y Postgrado; Argentina. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; ArgentinaFil: Monks, Sarah. National Center For Atmospheric Research. Amospheric Chemistry División; Estados Unidos. University of Colorado Boulder; Estados UnidosFil: Feng, Wuhu. University of Leeds; Reino UnidoFil: Brauer, Peter. University of New York; Estados Unidos. University of East Anglia; Reino UnidoFil: Von Glasow, Roland. University of East Anglia; Reino UnidoAmerican Geophysical Union2016-12info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/100772Hossaini, Ryan; Chipperfield, Martyn P.; Saiz Lopez, Alfonso; Fernandez, Rafael Pedro; Monks, Sarah; et al.; A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation; American Geophysical Union; Journal of Geophysical Research; 121; 23; 12-2016; 14.271-14.2970148-0227CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://onlinelibrary.wiley.com/doi/10.1002/2016JD025756/abstractinfo:eu-repo/semantics/altIdentifier/doi/10.1002/2016JD025756info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T15:08:18Zoai:ri.conicet.gov.ar:11336/100772instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-10-15 15:08:18.845CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation
title A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation
spellingShingle A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation
Hossaini, Ryan
TROPOSPHERIC CHLORINE
METHANE OXIDATION
VSL CHEMISTRY
title_short A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation
title_full A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation
title_fullStr A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation
title_full_unstemmed A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation
title_sort A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation
dc.creator.none.fl_str_mv Hossaini, Ryan
Chipperfield, Martyn P.
Saiz Lopez, Alfonso
Fernandez, Rafael Pedro
Monks, Sarah
Feng, Wuhu
Brauer, Peter
Von Glasow, Roland
author Hossaini, Ryan
author_facet Hossaini, Ryan
Chipperfield, Martyn P.
Saiz Lopez, Alfonso
Fernandez, Rafael Pedro
Monks, Sarah
Feng, Wuhu
Brauer, Peter
Von Glasow, Roland
author_role author
author2 Chipperfield, Martyn P.
Saiz Lopez, Alfonso
Fernandez, Rafael Pedro
Monks, Sarah
Feng, Wuhu
Brauer, Peter
Von Glasow, Roland
author2_role author
author
author
author
author
author
author
dc.subject.none.fl_str_mv TROPOSPHERIC CHLORINE
METHANE OXIDATION
VSL CHEMISTRY
topic TROPOSPHERIC CHLORINE
METHANE OXIDATION
VSL CHEMISTRY
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.5
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Chlorine atoms (Cl) are highly reactive toward hydrocarbons in the Earth’s troposphere, including the greenhouse gas methane (CH4). However, the regional and global CH4 sink from Cl is poorly quantified as tropospheric Cl concentrations ([Cl]) are uncertain by ~2 orders of magnitude. Here we describe the addition of a detailed tropospheric chlorine scheme to the TOMCAT chemical transport model. The model includes several sources of tropospheric inorganic chlorine (Cly), including (i) the oxidation of chlorocarbons of natural (CH3Cl, CHBr2Cl, CH2BrCl, and CHBrCl2) and anthropogenic (CH2Cl2, CHCl3, C2Cl4, C2HCl3, and CH2ClCH2Cl) origin and (ii) sea-salt aerosol dechlorination. Simulations were performed to quantify tropospheric [Cl], with a focus on the marine boundary layer, and quantify the global significance of Cl atom CH4 oxidation. In agreement with observations, simulated surface levels of hydrogen chloride (HCl), the most abundant Cly reservoir, reach several parts per billion (ppb) over polluted coastal/continental regions, with sub-ppb levels typical in more remote regions. Modeled annual mean surface [Cl] exhibits large spatial variability with the largest levels, typically in the range of 1-5×104 atoms cm-3, in the polluted northern hemisphere. Chlorocarbon oxidation provides a tropospheric Cly source of up to ~4320 Gg Cl/yr, sustaining a background surface [Cl] of <0.1 to 0.5 × 103 atoms cm-3 over large areas. Globally, we estimate a tropospheric methane sink of ~12-13 Tg CH4/yr due the CH4 + Cl reaction (~2.5% of total CH4 oxidation). Larger regional effects are predicted, with Cl accounting for ~10 to >20% of total boundary layer CH4 oxidation in some locations.
Fil: Hossaini, Ryan. University of Lancaster; Reino Unido
Fil: Chipperfield, Martyn P.. University of Leeds; Reino Unido
Fil: Saiz Lopez, Alfonso. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; España
Fil: Fernandez, Rafael Pedro. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; España. Universidad Tecnologica Nacional. Facultad Regional Mendoza. Secretaría de Ciencia, Tecnología y Postgrado; Argentina. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina
Fil: Monks, Sarah. National Center For Atmospheric Research. Amospheric Chemistry División; Estados Unidos. University of Colorado Boulder; Estados Unidos
Fil: Feng, Wuhu. University of Leeds; Reino Unido
Fil: Brauer, Peter. University of New York; Estados Unidos. University of East Anglia; Reino Unido
Fil: Von Glasow, Roland. University of East Anglia; Reino Unido
description Chlorine atoms (Cl) are highly reactive toward hydrocarbons in the Earth’s troposphere, including the greenhouse gas methane (CH4). However, the regional and global CH4 sink from Cl is poorly quantified as tropospheric Cl concentrations ([Cl]) are uncertain by ~2 orders of magnitude. Here we describe the addition of a detailed tropospheric chlorine scheme to the TOMCAT chemical transport model. The model includes several sources of tropospheric inorganic chlorine (Cly), including (i) the oxidation of chlorocarbons of natural (CH3Cl, CHBr2Cl, CH2BrCl, and CHBrCl2) and anthropogenic (CH2Cl2, CHCl3, C2Cl4, C2HCl3, and CH2ClCH2Cl) origin and (ii) sea-salt aerosol dechlorination. Simulations were performed to quantify tropospheric [Cl], with a focus on the marine boundary layer, and quantify the global significance of Cl atom CH4 oxidation. In agreement with observations, simulated surface levels of hydrogen chloride (HCl), the most abundant Cly reservoir, reach several parts per billion (ppb) over polluted coastal/continental regions, with sub-ppb levels typical in more remote regions. Modeled annual mean surface [Cl] exhibits large spatial variability with the largest levels, typically in the range of 1-5×104 atoms cm-3, in the polluted northern hemisphere. Chlorocarbon oxidation provides a tropospheric Cly source of up to ~4320 Gg Cl/yr, sustaining a background surface [Cl] of <0.1 to 0.5 × 103 atoms cm-3 over large areas. Globally, we estimate a tropospheric methane sink of ~12-13 Tg CH4/yr due the CH4 + Cl reaction (~2.5% of total CH4 oxidation). Larger regional effects are predicted, with Cl accounting for ~10 to >20% of total boundary layer CH4 oxidation in some locations.
publishDate 2016
dc.date.none.fl_str_mv 2016-12
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/100772
Hossaini, Ryan; Chipperfield, Martyn P.; Saiz Lopez, Alfonso; Fernandez, Rafael Pedro; Monks, Sarah; et al.; A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation; American Geophysical Union; Journal of Geophysical Research; 121; 23; 12-2016; 14.271-14.297
0148-0227
CONICET Digital
CONICET
url http://hdl.handle.net/11336/100772
identifier_str_mv Hossaini, Ryan; Chipperfield, Martyn P.; Saiz Lopez, Alfonso; Fernandez, Rafael Pedro; Monks, Sarah; et al.; A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation; American Geophysical Union; Journal of Geophysical Research; 121; 23; 12-2016; 14.271-14.297
0148-0227
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://onlinelibrary.wiley.com/doi/10.1002/2016JD025756/abstract
info:eu-repo/semantics/altIdentifier/doi/10.1002/2016JD025756
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Geophysical Union
publisher.none.fl_str_mv American Geophysical Union
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 13.22299

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