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

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Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic. / van Herpen, Maarten M.J.W.; Li, Qinyi; Saiz-Lopez, Alfonso; Liisberg, Jesper B.; Röckmann, Thomas; Cuevas, Carlos A.; Fernandez, Rafael P.; Mak, John E.; Mahowald, Natalie M.; Hess, Peter; Meidan, Daphne; Stuut, Jan Berend W.; Johnson, Matthew S.

I: Proceedings of the National Academy of Sciences of the United States of America, Bind 120, Nr. 31, e2303974120, 01.08.2023.

Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt

Harvard

van Herpen, MMJW, Li, Q, Saiz-Lopez, A, Liisberg, JB, Röckmann, T, Cuevas, CA, Fernandez, RP, Mak, JE, Mahowald, NM, Hess, P, Meidan, D, Stuut, JBW & Johnson, MS 2023, 'Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic', Proceedings of the National Academy of Sciences of the United States of America, bind 120, nr. 31, e2303974120. https://doi.org/10.1073/PNAS.2303974120

APA

van Herpen, M. M. J. W., Li, Q., Saiz-Lopez, A., Liisberg, J. B., Röckmann, T., Cuevas, C. A., Fernandez, R. P., Mak, J. E., Mahowald, N. M., Hess, P., Meidan, D., Stuut, J. B. W., & Johnson, M. S. (2023). Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic. Proceedings of the National Academy of Sciences of the United States of America, 120(31), [e2303974120]. https://doi.org/10.1073/PNAS.2303974120

Vancouver

van Herpen MMJW, Li Q, Saiz-Lopez A, Liisberg JB, Röckmann T, Cuevas CA o.a. Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic. Proceedings of the National Academy of Sciences of the United States of America. 2023 aug. 1;120(31). e2303974120. https://doi.org/10.1073/PNAS.2303974120

Author

van Herpen, Maarten M.J.W. ; Li, Qinyi ; Saiz-Lopez, Alfonso ; Liisberg, Jesper B. ; Röckmann, Thomas ; Cuevas, Carlos A. ; Fernandez, Rafael P. ; Mak, John E. ; Mahowald, Natalie M. ; Hess, Peter ; Meidan, Daphne ; Stuut, Jan Berend W. ; Johnson, Matthew S. / Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic. I: Proceedings of the National Academy of Sciences of the United States of America. 2023 ; Bind 120, Nr. 31.

Bibtex

@article{b90ff0e4be5a4258b15db7a39f417caa,
title = "Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic",
abstract = "Active chlorine in the atmosphere is poorly constrained and so is its role in the oxidation of the potent greenhouse gas methane, causing uncertainty in global methane budgets. We propose a photocatalytic mechanism for chlorine atom production that occurs when Sahara dust mixes with sea spray aerosol. The mechanism is validated by implementation 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)], which remained unexplained for decades. The production of Cl can also explain the anomaly in 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. Lawler et al., Atmos. Chem. Phys. 11, 7617–7628 (2011)]. Our model finds that 3.8 Tg(Cl) y−1 is produced over the North Atlantic, making it the dominant source of chlorine in the region; globally, chlorine production increases by 41%. The shift in the methane sink budget 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 biological sources such as agriculture and wetlands. Since 2014, an increase in North African dust emissions has increased the 13C isotope of atmospheric CH4, thereby partially masking a much greater decline in this isotope, which has implications for the interpretation of the drivers behind the recent increase of methane in the atmosphere.",
keywords = "aerosol chemistry, chemistry–climate, isotope modeling, methane removal, tropospheric chlorine",
author = "{van Herpen}, {Maarten M.J.W.} and Qinyi Li and Alfonso Saiz-Lopez and Liisberg, {Jesper B.} and Thomas R{\"o}ckmann and Cuevas, {Carlos A.} and Fernandez, {Rafael P.} and Mak, {John E.} and Mahowald, {Natalie M.} and Peter Hess and Daphne Meidan and Stuut, {Jan Berend W.} and Johnson, {Matthew S.}",
note = "Funding Information: ACKNOWLEDGMENTS. We thank Alex Wong for helpful comments and discussion. The CESM project is supported primarily by the NSF. Computing resources, support, and data storage were provided by the Climate Simulation Laboratory at NCAR{\textquoteright}s Computational and Information Systems Laboratory, sponsored by the NSF. Spark Climate Solutions: M.M.J.W.v.H., A.S.-L., J.B.L., T.R., and M.S.J. ACTRIS-DK: M.S.J. SilverLining: J.B.L., N.M.M., and M.S.J. European Research Council Executive Agency under the European Union{\textquoteright}s Horizon 2020 Research and Innovation Programme (Project ERC-2016-COG 726349 CLIMAHAL: A.S.-L.). Publisher Copyright: Copyright {\textcopyright} 2023 the Author(s).",
year = "2023",
month = aug,
day = "1",
doi = "10.1073/PNAS.2303974120",
language = "English",
volume = "120",
journal = "Proceedings of the National Academy of Sciences of the United States of America",
issn = "0027-8424",
publisher = "The National Academy of Sciences of the United States of America",
number = "31",

}

RIS

TY - JOUR

T1 - Photocatalytic chlorine atom production on mineral dust–sea spray aerosols over the North Atlantic

AU - van Herpen, Maarten M.J.W.

AU - Li, Qinyi

AU - Saiz-Lopez, Alfonso

AU - Liisberg, Jesper B.

AU - Röckmann, Thomas

AU - Cuevas, Carlos A.

AU - Fernandez, Rafael P.

AU - Mak, John E.

AU - Mahowald, Natalie M.

AU - Hess, Peter

AU - Meidan, Daphne

AU - Stuut, Jan Berend W.

AU - Johnson, Matthew S.

N1 - Funding Information: ACKNOWLEDGMENTS. We thank Alex Wong for helpful comments and discussion. The CESM project is supported primarily by the NSF. Computing resources, support, and data storage were provided by the Climate Simulation Laboratory at NCAR’s Computational and Information Systems Laboratory, sponsored by the NSF. Spark Climate Solutions: M.M.J.W.v.H., A.S.-L., J.B.L., T.R., and M.S.J. ACTRIS-DK: M.S.J. SilverLining: J.B.L., N.M.M., and M.S.J. European Research Council Executive Agency under the European Union’s Horizon 2020 Research and Innovation Programme (Project ERC-2016-COG 726349 CLIMAHAL: A.S.-L.). Publisher Copyright: Copyright © 2023 the Author(s).

PY - 2023/8/1

Y1 - 2023/8/1

N2 - Active chlorine in the atmosphere is poorly constrained and so is its role in the oxidation of the potent greenhouse gas methane, causing uncertainty in global methane budgets. We propose a photocatalytic mechanism for chlorine atom production that occurs when Sahara dust mixes with sea spray aerosol. The mechanism is validated by implementation 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)], which remained unexplained for decades. The production of Cl can also explain the anomaly in 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. Lawler et al., Atmos. Chem. Phys. 11, 7617–7628 (2011)]. Our model finds that 3.8 Tg(Cl) y−1 is produced over the North Atlantic, making it the dominant source of chlorine in the region; globally, chlorine production increases by 41%. The shift in the methane sink budget 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 biological sources such as agriculture and wetlands. Since 2014, an increase in North African dust emissions has increased the 13C isotope of atmospheric CH4, thereby partially masking a much greater decline in this isotope, which has implications for the interpretation of the drivers behind the recent increase of methane in the atmosphere.

AB - Active chlorine in the atmosphere is poorly constrained and so is its role in the oxidation of the potent greenhouse gas methane, causing uncertainty in global methane budgets. We propose a photocatalytic mechanism for chlorine atom production that occurs when Sahara dust mixes with sea spray aerosol. The mechanism is validated by implementation 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)], which remained unexplained for decades. The production of Cl can also explain the anomaly in 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. Lawler et al., Atmos. Chem. Phys. 11, 7617–7628 (2011)]. Our model finds that 3.8 Tg(Cl) y−1 is produced over the North Atlantic, making it the dominant source of chlorine in the region; globally, chlorine production increases by 41%. The shift in the methane sink budget 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 biological sources such as agriculture and wetlands. Since 2014, an increase in North African dust emissions has increased the 13C isotope of atmospheric CH4, thereby partially masking a much greater decline in this isotope, which has implications for the interpretation of the drivers behind the recent increase of methane in the atmosphere.

KW - aerosol chemistry

KW - chemistry–climate

KW - isotope modeling

KW - methane removal

KW - tropospheric chlorine

U2 - 10.1073/PNAS.2303974120

DO - 10.1073/PNAS.2303974120

M3 - Journal article

C2 - 37487065

AN - SCOPUS:85165662410

VL - 120

JO - Proceedings of the National Academy of Sciences of the United States of America

JF - Proceedings of the National Academy of Sciences of the United States of America

SN - 0027-8424

IS - 31

M1 - e2303974120

ER -

ID: 371560349