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

AuthorsHossaini, R.; Chipperfield, M.P.; Saiz-Lopez, A. ; Fernández, Rafael P.; Monks, S.; Feng, W.; Brauer, P.; Glasow, Roland
Issue Date2016
PublisherAmerican Geophysical Union
CitationJournal of Geophysical Research: Atmospheres 121: 14,271- 14,297 (2016)
AbstractChlorine atoms (Cl) are highly reactive toward hydrocarbons in the Earth's troposphere, including the greenhouse gas methane (CH). However, the regional and global CH 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 (Cl), including (i) the oxidation of chlorocarbons of natural (CHCl, CHBrCl, CHBrCl, and CHBrCl) and anthropogenic (CHCl, CHCl, CCl, CHCl, and CHClCHCl) 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 CH oxidation. In agreement with observations, simulated surface levels of hydrogen chloride (HCl), the most abundant Cl 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 × 10 atoms cm, 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 × 10 atoms cm over large areas. Globally, we estimate a tropospheric methane sink of ~12–13 Tg CH/yr due the CH + Cl reaction (~2.5% of total CH oxidation). Larger regional effects are predicted, with Cl accounting for ~10 to >20% of total boundary layer CH oxidation in some locations.
Identifiersdoi: 10.1002/2016JD025756
issn: 2169-8996
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