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Anthropogenic Impacts on Tropospheric Reactive Chlorine Since the Preindustrial

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Author(s)

  • Shuting Zhai
  • Xuan Wang
  • Joseph R. McConnell
  • Lei Geng
  • Jihong Cole-Dai
  • Michael Sigl
  • Nathan Chellman
  • Tomás Sherwen
  • Ryan Pound
  • Koji Fujita
  • Shohei Hattori
  • Jonathan M. Moch
  • Lei Zhu
  • Mat Evans
  • Michel Legrand
  • Pengfei Liu
  • Daniel Pasteris
  • Yuk Chun Chan
  • Lee T. Murray
  • Becky Alexander

Department/unit(s)

Publication details

JournalGeophysical Research Letters
DateAccepted/In press - 19 Jun 2021
DatePublished (current) - 28 Jul 2021
Issue number14
Volume48
Original languageEnglish

Abstract

Tropospheric reactive gaseous chlorine (Cly) impacts the atmosphere's oxidation capacity with implications for chemically reduced gases such as methane. Here we use Greenland ice-core records of chlorine, sodium, and acidity, and global model simulations to show how tropospheric Cly has been impacted by anthropogenic emissions since the 1940s. We show that anthropogenic contribution of nonsea-salt chlorine significantly influenced total chlorine and its trends after the 1940s. The modeled regional 170% Cly increase from preindustrial to the 1970s was driven by acid displacement from sea-salt-aerosol, direct emission of hydrochloric acid (HCl) from combustion, and chemical reactions driven by anthropogenic nitrogen oxide (NOx) emissions. Since the 1970s, the modeled 6% Cly decrease was caused mainly by reduced anthropogenic HCl emissions from air pollution mitigation policies. Our findings suggest that anthropogenic emissions of acidic gases and their emission control strategies have substantial impacts on Cly with implications for tropospheric oxidants, methane, and mercury.

Bibliographical note

Funding Information:
Becky Alexander, Shuting Zhai, and Yuk-Chun Chan acknowledge support from U.S. National Science Foundation (NSF) grants 1702266, 1644998, and 1904128. Shohei Hattori acknowledges support from MEXT/JSPS KAKENHI Grants JP16H05884 and JP20H04305. For Summit07, ice-core collection, analysis, and interpretation were supported by NSF Grants 0612461 and 0839066 to Jihong Cole-Dai. Lei Geng acknowledges support from the National Natural Science Foundation of China (Awards: 41822605). For all other ice cores, Joseph R. McConnell acknowledges support from NSF grants 0909541, 1023672, 1204176, and 1702830. The authors also thank the Danish-led North Greenland Eemian Ice Drilling (NEEM) consortium, the Alfred Wegener Institute, the U.S. Ice Drilling Program, as well as staff and students of the DRI ice core laboratory including O. Maselli, and L. Layman. Shuting Zhai acknowledges fruitful discussions with L. Jaegl?, H. Horowitz, J. Huang, V. Shah, J. Shao, and Q. Chen.

Funding Information:
Becky Alexander, Shuting Zhai, and Yuk‐Chun Chan acknowledge support from U.S. National Science Foundation (NSF) grants 1702266, 1644998, and 1904128. Shohei Hattori acknowledges support from MEXT/JSPS KAKENHI Grants JP16H05884 and JP20H04305. For Summit07, ice‐core collection, analysis, and interpretation were supported by NSF Grants 0612461 and 0839066 to Jihong Cole‐Dai. Lei Geng acknowledges support from the National Natural Science Foundation of China (Awards: 41822605). For all other ice cores, Joseph R. McConnell acknowledges support from NSF grants 0909541, 1023672, 1204176, and 1702830. The authors also thank the Danish‐led North Greenland Eemian Ice Drilling (NEEM) consortium, the Alfred Wegener Institute, the U.S. Ice Drilling Program, as well as staff and students of the DRI ice core laboratory including O. Maselli, and L. Layman. Shuting Zhai acknowledges fruitful discussions with L. Jaeglé, H. Horowitz, J. Huang, V. Shah, J. Shao, and Q. Chen.

Publisher Copyright:
© 2021. American Geophysical Union. All Rights Reserved.

    Research areas

  • chlorine, halogens, icecores, modelling, observations

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