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A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation

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A global model of tropospheric chlorine chemistry : Organic versus inorganic sources and impact on methane oxidation. / Hossaini, Ryan; Chipperfield, Martyn P.; Saiz-Lopez, Alfonso; Fernandez, Rafael P.; Monks, Sarah; Feng, Wuhu; Brauer, Peter; Von Glasow, Roland.

In: Journal of Geophysical Research G: Biogeosciences, Vol. 121, No. 23, 16.12.2016, p. 14,271-14,297.

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Harvard

Hossaini, R, Chipperfield, MP, Saiz-Lopez, A, Fernandez, RP, Monks, S, Feng, W, Brauer, P & Von Glasow, R 2016, 'A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation', Journal of Geophysical Research G: Biogeosciences, vol. 121, no. 23, pp. 14,271-14,297. https://doi.org/10.1002/2016JD025756

APA

Hossaini, R., Chipperfield, M. P., Saiz-Lopez, A., Fernandez, R. P., Monks, S., Feng, W., ... Von Glasow, R. (2016). A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation. Journal of Geophysical Research G: Biogeosciences, 121(23), 14,271-14,297. https://doi.org/10.1002/2016JD025756

Vancouver

Hossaini R, Chipperfield MP, Saiz-Lopez A, Fernandez RP, Monks S, Feng W et al. A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation. Journal of Geophysical Research G: Biogeosciences. 2016 Dec 16;121(23):14,271-14,297. https://doi.org/10.1002/2016JD025756

Author

Hossaini, Ryan ; Chipperfield, Martyn P. ; Saiz-Lopez, Alfonso ; Fernandez, Rafael P. ; Monks, Sarah ; Feng, Wuhu ; Brauer, Peter ; Von Glasow, Roland. / A global model of tropospheric chlorine chemistry : Organic versus inorganic sources and impact on methane oxidation. In: Journal of Geophysical Research G: Biogeosciences. 2016 ; Vol. 121, No. 23. pp. 14,271-14,297.

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@article{839efcf7b4b8481fa8185a2702af7d5f,
title = "A global model of tropospheric chlorine chemistry: Organic versus inorganic sources and impact on methane oxidation",
abstract = "Chlorine atoms (Cl) are highly reactive toward hydrocarbons in the Earth’s troposphere, including the greenhouse gas methane (CH4). However, the regional and global CH4 sink from Cl is poorly quantified as tropospheric Cl concentrations ([Cl]) are uncertain by ~2 orders of magnitude. Here we describe the addition of a detailed tropospheric chlorine scheme to the TOMCAT chemical transport model. The model includes several sources of tropospheric inorganic chlorine (Cly), including (i) the oxidation of chlorocarbons of natural (CH3Cl, CHBr2Cl, CH2BrCl, and CHBrCl2) and anthropogenic (CH2Cl2, CHCl3, C2Cl4, C2HCl3, and CH2ClCH2Cl) origin and (ii) sea-salt aerosol dechlorination. Simulations were performed to quantify tropospheric [Cl], with a focus on the marine boundary layer, and quantify the global significance of Cl atom CH4 oxidation. In agreement with observations, simulated surface levels of hydrogen chloride (HCl), the most abundant Cly reservoir, reach several parts per billion (ppb) over polluted coastal/continental regions, with sub-ppb levels typical in more remote regions. Modeled annual mean surface [Cl] exhibits large spatial variability with the largest levels, typically in the range of 1-5×104 atoms cm-3, in the polluted northern hemisphere. Chlorocarbon oxidation provides a tropospheric Cly source of up to ~4320 Gg Cl/yr, sustaining a background surface [Cl] of <0.1 to 0.5 × 103 atoms cm-3 over large areas. Globally, we estimate a tropospheric methane sink of ~12-13 Tg CH4/yr due the CH4 + Cl reaction (~2.5{\%} of total CH4 oxidation). Larger regional effects are predicted, with Cl accounting for ~10 to >20{\%} of total boundary layer CH4 oxidation in some locations.",
author = "Ryan Hossaini and Chipperfield, {Martyn P.} and Alfonso Saiz-Lopez and Fernandez, {Rafael P.} and Sarah Monks and Wuhu Feng and Peter Brauer and {Von Glasow}, Roland",
note = "{\circledC}2016. The Authors.",
year = "2016",
month = "12",
day = "16",
doi = "10.1002/2016JD025756",
language = "English",
volume = "121",
pages = "14,271--14,297",
journal = "Journal of Geophysical Research G: Biogeosciences",
issn = "2169-8953",
publisher = "Wiley-Blackwell",
number = "23",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - A global model of tropospheric chlorine chemistry

T2 - Organic versus inorganic sources and impact on methane oxidation

AU - Hossaini, Ryan

AU - Chipperfield, Martyn P.

AU - Saiz-Lopez, Alfonso

AU - Fernandez, Rafael P.

AU - Monks, Sarah

AU - Feng, Wuhu

AU - Brauer, Peter

AU - Von Glasow, Roland

N1 - ©2016. The Authors.

PY - 2016/12/16

Y1 - 2016/12/16

N2 - Chlorine atoms (Cl) are highly reactive toward hydrocarbons in the Earth’s troposphere, including the greenhouse gas methane (CH4). However, the regional and global CH4 sink from Cl is poorly quantified as tropospheric Cl concentrations ([Cl]) are uncertain by ~2 orders of magnitude. Here we describe the addition of a detailed tropospheric chlorine scheme to the TOMCAT chemical transport model. The model includes several sources of tropospheric inorganic chlorine (Cly), including (i) the oxidation of chlorocarbons of natural (CH3Cl, CHBr2Cl, CH2BrCl, and CHBrCl2) and anthropogenic (CH2Cl2, CHCl3, C2Cl4, C2HCl3, and CH2ClCH2Cl) origin and (ii) sea-salt aerosol dechlorination. Simulations were performed to quantify tropospheric [Cl], with a focus on the marine boundary layer, and quantify the global significance of Cl atom CH4 oxidation. In agreement with observations, simulated surface levels of hydrogen chloride (HCl), the most abundant Cly reservoir, reach several parts per billion (ppb) over polluted coastal/continental regions, with sub-ppb levels typical in more remote regions. Modeled annual mean surface [Cl] exhibits large spatial variability with the largest levels, typically in the range of 1-5×104 atoms cm-3, in the polluted northern hemisphere. Chlorocarbon oxidation provides a tropospheric Cly source of up to ~4320 Gg Cl/yr, sustaining a background surface [Cl] of <0.1 to 0.5 × 103 atoms cm-3 over large areas. Globally, we estimate a tropospheric methane sink of ~12-13 Tg CH4/yr due the CH4 + Cl reaction (~2.5% of total CH4 oxidation). Larger regional effects are predicted, with Cl accounting for ~10 to >20% of total boundary layer CH4 oxidation in some locations.

AB - Chlorine atoms (Cl) are highly reactive toward hydrocarbons in the Earth’s troposphere, including the greenhouse gas methane (CH4). However, the regional and global CH4 sink from Cl is poorly quantified as tropospheric Cl concentrations ([Cl]) are uncertain by ~2 orders of magnitude. Here we describe the addition of a detailed tropospheric chlorine scheme to the TOMCAT chemical transport model. The model includes several sources of tropospheric inorganic chlorine (Cly), including (i) the oxidation of chlorocarbons of natural (CH3Cl, CHBr2Cl, CH2BrCl, and CHBrCl2) and anthropogenic (CH2Cl2, CHCl3, C2Cl4, C2HCl3, and CH2ClCH2Cl) origin and (ii) sea-salt aerosol dechlorination. Simulations were performed to quantify tropospheric [Cl], with a focus on the marine boundary layer, and quantify the global significance of Cl atom CH4 oxidation. In agreement with observations, simulated surface levels of hydrogen chloride (HCl), the most abundant Cly reservoir, reach several parts per billion (ppb) over polluted coastal/continental regions, with sub-ppb levels typical in more remote regions. Modeled annual mean surface [Cl] exhibits large spatial variability with the largest levels, typically in the range of 1-5×104 atoms cm-3, in the polluted northern hemisphere. Chlorocarbon oxidation provides a tropospheric Cly source of up to ~4320 Gg Cl/yr, sustaining a background surface [Cl] of <0.1 to 0.5 × 103 atoms cm-3 over large areas. Globally, we estimate a tropospheric methane sink of ~12-13 Tg CH4/yr due the CH4 + Cl reaction (~2.5% of total CH4 oxidation). Larger regional effects are predicted, with Cl accounting for ~10 to >20% of total boundary layer CH4 oxidation in some locations.

UR - http://www.scopus.com/inward/record.url?scp=85007270904&partnerID=8YFLogxK

U2 - 10.1002/2016JD025756

DO - 10.1002/2016JD025756

M3 - Article

VL - 121

SP - 14,271-14,297

JO - Journal of Geophysical Research G: Biogeosciences

JF - Journal of Geophysical Research G: Biogeosciences

SN - 2169-8953

IS - 23

ER -