Anthropogenic Impacts on Tropospheric Reactive Chlorine Since the Preindustrial

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

doi:10.1029/2021GL093808

Anthropogenic Impacts on Tropospheric Reactive Chlorine Since the Preindustrial

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^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

Abstract

Tropospheric reactive gaseous chlorine (Cl_y) 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 Cl_y 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% Cl_y 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 (NO_x) emissions. Since the 1970s, the modeled 6% Cl_y 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 Cl_y with implications for tropospheric oxidants, methane, and mercury.

Original language	English
Article number	e2021GL093808
Journal	Geophysical Research Letters
Volume	48
Issue number	14
DOIs	https://doi.org/10.1029/2021GL093808
Publication status	Published - 28 Jul 2021

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.

Keywords

chlorine
halogens
icecores
modelling
observations

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10.1029/2021GL093808

2021GL093808
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Zhai, S., Wang, X., McConnell, J. R., Geng, L., Cole-Dai, J., Sigl, M., Chellman, N., Sherwen, T., Pound, R., Fujita, K., Hattori, S., Moch, J. M., Zhu, L., Evans, M., Legrand, M., Liu, P., Pasteris, D., Chan, Y. C., Murray, L. T., & Alexander, B. (2021). Anthropogenic Impacts on Tropospheric Reactive Chlorine Since the Preindustrial. Geophysical Research Letters, 48(14), Article e2021GL093808. https://doi.org/10.1029/2021GL093808

@article{154b0aa4789f41d381a546135fceb229,

title = "Anthropogenic Impacts on Tropospheric Reactive Chlorine Since the Preindustrial",

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.",

keywords = "chlorine, halogens, icecores, modelling, observations",

author = "Shuting Zhai and Xuan Wang and McConnell, {Joseph R.} and Lei Geng and Jihong Cole-Dai and Michael Sigl and Nathan Chellman and Tom{\'a}s Sherwen and Ryan Pound and Koji Fujita and Shohei Hattori and Moch, {Jonathan M.} and Lei Zhu and Mat Evans and Michel Legrand and Pengfei Liu and Daniel Pasteris and Chan, {Yuk Chun} and Murray, {Lee T.} and Becky Alexander",

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. Jaegl{\'e}, H. Horowitz, J. Huang, V. Shah, J. Shao, and Q. Chen. Publisher Copyright: {\textcopyright} 2021. American Geophysical Union. All Rights Reserved.",

year = "2021",

month = jul,

day = "28",

doi = "10.1029/2021GL093808",

language = "English",

volume = "48",

journal = "Geophysical Research Letters",

issn = "0094-8276",

publisher = "American Geophysical Union",

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Zhai, S, Wang, X, McConnell, JR, Geng, L, Cole-Dai, J, Sigl, M, Chellman, N, Sherwen, T , Pound, R, Fujita, K, Hattori, S, Moch, JM, Zhu, L, Evans, M, Legrand, M, Liu, P, Pasteris, D, Chan, YC, Murray, LT & Alexander, B 2021, 'Anthropogenic Impacts on Tropospheric Reactive Chlorine Since the Preindustrial', Geophysical Research Letters, vol. 48, no. 14, e2021GL093808. https://doi.org/10.1029/2021GL093808

TY - JOUR

T1 - Anthropogenic Impacts on Tropospheric Reactive Chlorine Since the Preindustrial

AU - Zhai, Shuting

AU - Wang, Xuan

AU - McConnell, Joseph R.

AU - Geng, Lei

AU - Cole-Dai, Jihong

AU - Sigl, Michael

AU - Chellman, Nathan

AU - Sherwen, Tomás

AU - Pound, Ryan

AU - Fujita, Koji

AU - Hattori, Shohei

AU - Moch, Jonathan M.

AU - Zhu, Lei

AU - Evans, Mat

AU - Legrand, Michel

AU - Liu, Pengfei

AU - Pasteris, Daniel

AU - Chan, Yuk Chun

AU - Murray, Lee T.

AU - Alexander, Becky

N1 - 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.

PY - 2021/7/28

Y1 - 2021/7/28

N2 - 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.

AB - 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.

KW - chlorine

KW - halogens

KW - icecores

KW - modelling

KW - observations

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U2 - 10.1029/2021GL093808

DO - 10.1029/2021GL093808

M3 - Article

SN - 0094-8276

VL - 48

JO - Geophysical Research Letters

JF - Geophysical Research Letters

IS - 14

M1 - e2021GL093808

ER -

Anthropogenic Impacts on Tropospheric Reactive Chlorine Since the Preindustrial

Abstract

Bibliographical note

Keywords

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