Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic

Autores
van Herpen, Maarten M. J. W.; Li, Qinyi; Saiz López, Alfonso; Liisberg, Jesper B.; Röckmann,Thomas; Cuevas Rodríguez, Carlos Alberto; Fernandez, Rafael Pedro; Mak, John E.; Mahowald, Natalie M.; Hess, Peter; Meidan, Daphne; Stuut, Jan-­Berend W.; Matthew S. Johnson
Año de publicación
2023
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Active chlorine in the atmosphere is poorly constrained and so is its role in the oxidationof the potent greenhouse gas methane, causing uncertainty in global methane budgets.We propose a photocatalytic mechanism for chlorine atom production that occurs whenSahara dust mixes with sea spray aerosol. The mechanism is validated by implemen-tation in a global atmospheric model and thereby explaining the episodic, seasonal,and location-­dependent 13C depletion in CO in air samples from Barbados [J.E. Mak,G. Kra, T. Sandomenico, P. Bergamaschi, J. Geophys. Res. Atmos. 108 (2003)], whichremained unexplained for decades. The production of Cl can also explain the anomalyin the CO:ethane ratio found at Cape Verde [K. A. Read et al., J. Geophys. Res. Atmos.114 (2009)], in addition to explaining the observation of elevated HOCl [M. J. Lawleret al., Atmos. Chem. Phys. 11, 7617–7628 (2011)]. Our model finds that 3.8 Tg(Cl) y−1is produced over the North Atlantic, making it the dominant source of chlorine in theregion; globally, chlorine production increases by 41%. The shift in the methane sinkbudget due to the increased role of Cl means that isotope-­constrained top–down models fail to allocate 12 Tg y−1 (2% of total methane emissions) to 13C-­depleted biologicalsources such as agriculture and wetlands. Since 2014, an increase in North African dustemissions has increased the 13C isotope of atmospheric CH4, thereby partially maskinga much greater decline in this isotope, which has implications for the interpretation ofthe drivers behind the recent increase of methane in the atmosphere.
Fil: van Herpen, Maarten M. J. W.. Acacia Impact Innovation; Países Bajos
Fil: Li, Qinyi. Consejo Superior de Investigaciones Científicas. Instituto de Química Física "Rocasolano"; España. Consejo Superior de Investigaciones Científicas. Instituto de Quimica Física Blas Cabrera. Departamento de Química Atmosférica y Clima. ; España
Fil: Saiz López, Alfonso. Consejo Superior de Investigaciones Científicas. Instituto de Quimica Física Blas Cabrera. Departamento de Química Atmosférica y Clima. ; España
Fil: Liisberg, Jesper B.. Universidad de Copenhagen; Dinamarca
Fil: Röckmann,Thomas. University of Utrecht; Países Bajos
Fil: Cuevas Rodríguez, Carlos Alberto. Consejo Superior de Investigaciones Científicas Instituto de Química Física Blas Cabrera. Departamento de Química Atmosférica y Clima; España
Fil: Fernandez, Rafael Pedro. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza. Instituto Interdisciplinario de Ciencias Básicas. - Universidad Nacional de Cuyo. Instituto Interdisciplinario de Ciencias Básicas; Argentina. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina
Fil: Mak, John E.. Stony Brook University ; State University Of New York;
Fil: Mahowald, Natalie M.. Cornell University; Estados Unidos
Fil: Hess, Peter. Cornell University; Estados Unidos
Fil: Meidan, Daphne. Cornell University; Estados Unidos
Fil: Stuut, Jan-­Berend W.. University of Amsterdam; Países Bajos. Royal Netherlands Institute for Sea Research; Países Bajos
Fil: Matthew S. Johnson. Universidad de Copenhagen; Dinamarca
Materia
METHANE REMOVAL
TROPOSPHERIC CHLORINE
CHEMISTRY-CLIMATE
AEROSOL-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:11336/245761
Acceder
id CONICETDig_d9c7642248c99d03319ee7dedcc07769
oai_identifier_str oai:ri.conicet.gov.ar:11336/245761
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlanticvan Herpen, Maarten M. J. W.Li, QinyiSaiz López, AlfonsoLiisberg, Jesper B.Röckmann,ThomasCuevas Rodríguez, Carlos AlbertoFernandez, Rafael PedroMak, John E.Mahowald, Natalie M.Hess, PeterMeidan, DaphneStuut, Jan-­Berend W.Matthew S. JohnsonMETHANE REMOVALTROPOSPHERIC CHLORINECHEMISTRY-CLIMATEAEROSOL-CHEMISTRYhttps://purl.org/becyt/ford/1.5https://purl.org/becyt/ford/1Active chlorine in the atmosphere is poorly constrained and so is its role in the oxidationof the potent greenhouse gas methane, causing uncertainty in global methane budgets.We propose a photocatalytic mechanism for chlorine atom production that occurs whenSahara dust mixes with sea spray aerosol. The mechanism is validated by implemen-tation in a global atmospheric model and thereby explaining the episodic, seasonal,and location-­dependent 13C depletion in CO in air samples from Barbados [J.E. Mak,G. Kra, T. Sandomenico, P. Bergamaschi, J. Geophys. Res. Atmos. 108 (2003)], whichremained unexplained for decades. The production of Cl can also explain the anomalyin the CO:ethane ratio found at Cape Verde [K. A. Read et al., J. Geophys. Res. Atmos.114 (2009)], in addition to explaining the observation of elevated HOCl [M. J. Lawleret al., Atmos. Chem. Phys. 11, 7617–7628 (2011)]. Our model finds that 3.8 Tg(Cl) y−1is produced over the North Atlantic, making it the dominant source of chlorine in theregion; globally, chlorine production increases by 41%. The shift in the methane sinkbudget due to the increased role of Cl means that isotope-­constrained top–down models fail to allocate 12 Tg y−1 (2% of total methane emissions) to 13C-­depleted biologicalsources such as agriculture and wetlands. Since 2014, an increase in North African dustemissions has increased the 13C isotope of atmospheric CH4, thereby partially maskinga much greater decline in this isotope, which has implications for the interpretation ofthe drivers behind the recent increase of methane in the atmosphere.Fil: van Herpen, Maarten M. J. W.. Acacia Impact Innovation; Países BajosFil: Li, Qinyi. Consejo Superior de Investigaciones Científicas. Instituto de Química Física "Rocasolano"; España. Consejo Superior de Investigaciones Científicas. Instituto de Quimica Física Blas Cabrera. Departamento de Química Atmosférica y Clima. ; EspañaFil: Saiz López, Alfonso. Consejo Superior de Investigaciones Científicas. Instituto de Quimica Física Blas Cabrera. Departamento de Química Atmosférica y Clima. ; EspañaFil: Liisberg, Jesper B.. Universidad de Copenhagen; DinamarcaFil: Röckmann,Thomas. University of Utrecht; Países BajosFil: Cuevas Rodríguez, Carlos Alberto. Consejo Superior de Investigaciones Científicas Instituto de Química Física Blas Cabrera. Departamento de Química Atmosférica y Clima; EspañaFil: Fernandez, Rafael Pedro. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza. Instituto Interdisciplinario de Ciencias Básicas. - Universidad Nacional de Cuyo. Instituto Interdisciplinario de Ciencias Básicas; Argentina. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; ArgentinaFil: Mak, John E.. Stony Brook University ; State University Of New York;Fil: Mahowald, Natalie M.. Cornell University; Estados UnidosFil: Hess, Peter. Cornell University; Estados UnidosFil: Meidan, Daphne. Cornell University; Estados UnidosFil: Stuut, Jan-­Berend W.. University of Amsterdam; Países Bajos. Royal Netherlands Institute for Sea Research; Países BajosFil: Matthew S. Johnson. Universidad de Copenhagen; DinamarcaNational Academy of Sciences2023-07-24info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/245761van Herpen, Maarten M. J. W.; Li, Qinyi; Saiz López, Alfonso; Liisberg, Jesper B.; Röckmann,Thomas; et al.; Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic; National Academy of Sciences; Proceedings of the National Academy of Sciences of The United States of America; 120; 31; 24-7-2023; 1 -81091-6490CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.pnas.org/doi/abs/10.1073/pnas.2303974120info:eu-repo/semantics/altIdentifier/doi/10.1073/PNAS.2303974120info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T14:30:18Zoai:ri.conicet.gov.ar:11336/245761instacron: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 14:30:18.408CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic
title Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic
spellingShingle Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic
van Herpen, Maarten M. J. W.
METHANE REMOVAL
TROPOSPHERIC CHLORINE
CHEMISTRY-CLIMATE
AEROSOL-CHEMISTRY
title_short Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic
title_full Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic
title_fullStr Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic
title_full_unstemmed Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic
title_sort Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic
dc.creator.none.fl_str_mv van Herpen, Maarten M. J. W.
Li, Qinyi
Saiz López, Alfonso
Liisberg, Jesper B.
Röckmann,Thomas
Cuevas Rodríguez, Carlos Alberto
Fernandez, Rafael Pedro
Mak, John E.
Mahowald, Natalie M.
Hess, Peter
Meidan, Daphne
Stuut, Jan-­Berend W.
Matthew S. Johnson
author van Herpen, Maarten M. J. W.
author_facet van Herpen, Maarten M. J. W.
Li, Qinyi
Saiz López, Alfonso
Liisberg, Jesper B.
Röckmann,Thomas
Cuevas Rodríguez, Carlos Alberto
Fernandez, Rafael Pedro
Mak, John E.
Mahowald, Natalie M.
Hess, Peter
Meidan, Daphne
Stuut, Jan-­Berend W.
Matthew S. Johnson
author_role author
author2 Li, Qinyi
Saiz López, Alfonso
Liisberg, Jesper B.
Röckmann,Thomas
Cuevas Rodríguez, Carlos Alberto
Fernandez, Rafael Pedro
Mak, John E.
Mahowald, Natalie M.
Hess, Peter
Meidan, Daphne
Stuut, Jan-­Berend W.
Matthew S. Johnson
author2_role author
author
author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv METHANE REMOVAL
TROPOSPHERIC CHLORINE
CHEMISTRY-CLIMATE
AEROSOL-CHEMISTRY
topic METHANE REMOVAL
TROPOSPHERIC CHLORINE
CHEMISTRY-CLIMATE
AEROSOL-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 Active chlorine in the atmosphere is poorly constrained and so is its role in the oxidationof the potent greenhouse gas methane, causing uncertainty in global methane budgets.We propose a photocatalytic mechanism for chlorine atom production that occurs whenSahara dust mixes with sea spray aerosol. The mechanism is validated by implemen-tation in a global atmospheric model and thereby explaining the episodic, seasonal,and location-­dependent 13C depletion in CO in air samples from Barbados [J.E. Mak,G. Kra, T. Sandomenico, P. Bergamaschi, J. Geophys. Res. Atmos. 108 (2003)], whichremained unexplained for decades. The production of Cl can also explain the anomalyin the CO:ethane ratio found at Cape Verde [K. A. Read et al., J. Geophys. Res. Atmos.114 (2009)], in addition to explaining the observation of elevated HOCl [M. J. Lawleret al., Atmos. Chem. Phys. 11, 7617–7628 (2011)]. Our model finds that 3.8 Tg(Cl) y−1is produced over the North Atlantic, making it the dominant source of chlorine in theregion; globally, chlorine production increases by 41%. The shift in the methane sinkbudget due to the increased role of Cl means that isotope-­constrained top–down models fail to allocate 12 Tg y−1 (2% of total methane emissions) to 13C-­depleted biologicalsources such as agriculture and wetlands. Since 2014, an increase in North African dustemissions has increased the 13C isotope of atmospheric CH4, thereby partially maskinga much greater decline in this isotope, which has implications for the interpretation ofthe drivers behind the recent increase of methane in the atmosphere.
Fil: van Herpen, Maarten M. J. W.. Acacia Impact Innovation; Países Bajos
Fil: Li, Qinyi. Consejo Superior de Investigaciones Científicas. Instituto de Química Física "Rocasolano"; España. Consejo Superior de Investigaciones Científicas. Instituto de Quimica Física Blas Cabrera. Departamento de Química Atmosférica y Clima. ; España
Fil: Saiz López, Alfonso. Consejo Superior de Investigaciones Científicas. Instituto de Quimica Física Blas Cabrera. Departamento de Química Atmosférica y Clima. ; España
Fil: Liisberg, Jesper B.. Universidad de Copenhagen; Dinamarca
Fil: Röckmann,Thomas. University of Utrecht; Países Bajos
Fil: Cuevas Rodríguez, Carlos Alberto. Consejo Superior de Investigaciones Científicas Instituto de Química Física Blas Cabrera. Departamento de Química Atmosférica y Clima; España
Fil: Fernandez, Rafael Pedro. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza. Instituto Interdisciplinario de Ciencias Básicas. - Universidad Nacional de Cuyo. Instituto Interdisciplinario de Ciencias Básicas; Argentina. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina
Fil: Mak, John E.. Stony Brook University ; State University Of New York;
Fil: Mahowald, Natalie M.. Cornell University; Estados Unidos
Fil: Hess, Peter. Cornell University; Estados Unidos
Fil: Meidan, Daphne. Cornell University; Estados Unidos
Fil: Stuut, Jan-­Berend W.. University of Amsterdam; Países Bajos. Royal Netherlands Institute for Sea Research; Países Bajos
Fil: Matthew S. Johnson. Universidad de Copenhagen; Dinamarca
description Active chlorine in the atmosphere is poorly constrained and so is its role in the oxidationof the potent greenhouse gas methane, causing uncertainty in global methane budgets.We propose a photocatalytic mechanism for chlorine atom production that occurs whenSahara dust mixes with sea spray aerosol. The mechanism is validated by implemen-tation in a global atmospheric model and thereby explaining the episodic, seasonal,and location-­dependent 13C depletion in CO in air samples from Barbados [J.E. Mak,G. Kra, T. Sandomenico, P. Bergamaschi, J. Geophys. Res. Atmos. 108 (2003)], whichremained unexplained for decades. The production of Cl can also explain the anomalyin the CO:ethane ratio found at Cape Verde [K. A. Read et al., J. Geophys. Res. Atmos.114 (2009)], in addition to explaining the observation of elevated HOCl [M. J. Lawleret al., Atmos. Chem. Phys. 11, 7617–7628 (2011)]. Our model finds that 3.8 Tg(Cl) y−1is produced over the North Atlantic, making it the dominant source of chlorine in theregion; globally, chlorine production increases by 41%. The shift in the methane sinkbudget due to the increased role of Cl means that isotope-­constrained top–down models fail to allocate 12 Tg y−1 (2% of total methane emissions) to 13C-­depleted biologicalsources such as agriculture and wetlands. Since 2014, an increase in North African dustemissions has increased the 13C isotope of atmospheric CH4, thereby partially maskinga much greater decline in this isotope, which has implications for the interpretation ofthe drivers behind the recent increase of methane in the atmosphere.
publishDate 2023
dc.date.none.fl_str_mv 2023-07-24
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/11336/245761
van Herpen, Maarten M. J. W.; Li, Qinyi; Saiz López, Alfonso; Liisberg, Jesper B.; Röckmann,Thomas; et al.; Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic; National Academy of Sciences; Proceedings of the National Academy of Sciences of The United States of America; 120; 31; 24-7-2023; 1 -8
1091-6490
CONICET Digital
CONICET
url http://hdl.handle.net/11336/245761
identifier_str_mv van Herpen, Maarten M. J. W.; Li, Qinyi; Saiz López, Alfonso; Liisberg, Jesper B.; Röckmann,Thomas; et al.; Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic; National Academy of Sciences; Proceedings of the National Academy of Sciences of The United States of America; 120; 31; 24-7-2023; 1 -8
1091-6490
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://www.pnas.org/doi/abs/10.1073/pnas.2303974120
info:eu-repo/semantics/altIdentifier/doi/10.1073/PNAS.2303974120
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 National Academy of Sciences
publisher.none.fl_str_mv National Academy of Sciences
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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