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

Author:

van Herpen Maarten M. J. W.1ORCID,Li Qinyi2ORCID,Saiz-Lopez Alfonso2ORCID,Liisberg Jesper B.3,Röckmann Thomas4ORCID,Cuevas Carlos A.2ORCID,Fernandez Rafael P.56ORCID,Mak John E.7ORCID,Mahowald Natalie M.8ORCID,Hess Peter9,Meidan Daphne8ORCID,Stuut Jan-Berend W.1011ORCID,Johnson Matthew S.3ORCID

Affiliation:

1. Acacia Impact Innovation, Maarten van Herpen, Bernheze 5384 BB, The Netherlands

2. Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Blas Cabrera, Spanish National Research Council, 28006 Madrid, Spain

3. Department of Chemistry, University of Copenhagen, DK-2100 Copenhagen Ø, Denmark

4. Institute for Marine and Atmospheric Research Utrecht, Department of Physics, Faculty of Science, Utrecht University, 3584 CS Utrecht, The Netherlands

5. Institute for Interdisciplinary Science, National Research Council, Mendoza 5501, Argentina

6. School of Natural Sciences, National University of Cuyo, Mendoza 5501, Argentina

7. School of Marine and Atmospheric Sciences, Stony Brook University, Brookhaven, NY 11790

8. Department of Earth and Atmospheric Sciences, Cornell University, Ithaca, NY 14853

9. Department of Biological and Environmental Engineering, Cornell University, Ithaca, NY 14853

10. Royal Netherlands Institute for Sea Research, Landsdiep 4, 1797 SZ, ‘t Horntje, The Netherlands

11. Department of Earth Sciences, Faculty of Science, Vrije Universiteit Amsterdam, 1105, Amsterdam, The Netherlands

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-dependent13C 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−1is 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) to13C-depleted biological sources such as agriculture and wetlands. Since 2014, an increase in North African dust emissions has increased the13C 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.

Funder

Spark Climate Solutions

ACTRIS-DK

Silver Lining

EC | ERC | HORIZON EUROPE European Research Council

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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