The EMEP/MSC-E mercury modeling system

Travnikov, Oleg; Ilyin, Ilia

doi:10.1007/978-0-387-93958-2_20

Cited by 54 publications

(38 citation statements)

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“…Previous studies have assumed O 3 and OH to be the major Hg 0 oxidants in the atmosphere [51][52][53][54][55][56]. Despite theoretical doubts concerning the thermal stability of gaseous HgOH and HgO products, many modeling results using O 3 /OH as the main atmospheric Hg oxidants showed good agreement with the observed Hg 0 concentration and wet deposition flux.…”

Section: Dominant Gaseous Oxidant For Hg 0 : O 3 /Oh Br or Others?mentioning

confidence: 69%

Recent Advances in Atmospheric Chemistry of Mercury

Ariya

2018

Atmosphere

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Mercury is one of the most toxic metals and has global importance due to the biomagnification and bioaccumulation of organomercury via the aquatic food web. The physical and chemical transformations of various mercury species in the atmosphere strongly influence their composition, phase, transport characteristics and deposition rate to the ground. Modeling efforts to evaluate the mercury cycling in the environment require an accurate understanding of atmospheric mercury chemistry. We focus this article on recent studies (since 2015) on improving our understanding of the atmospheric chemistry of mercury. We discuss recent advances in (i) determining the dominant atmospheric oxidant of elemental mercury (Hg 0 ); (ii) understanding the oxidation reactions of Hg 0 by halogen atoms and by nitrate radical (NO 3 ); (iii) the aqueous reduction of oxidized mercury compounds (Hg II ); and (iv) the heterogeneous reactions of Hg on atmospherically-relevant surfaces. The need for future research to improve understanding of the fate and transformation of mercury in the atmosphere is also discussed.

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Section: Dominant Gaseous Oxidant For Hg 0 : O 3 /Oh Br or Others?mentioning

confidence: 69%

Recent Advances in Atmospheric Chemistry of Mercury

Ariya

2018

Atmosphere

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“…GLEMOS is a multi-scale chemistry transport model developed for the simulation of environmental dispersion and cycling of different chemicals, including mercury, based on the older hemispheric model MSCE-HM-Hem (Travnikov, 2005;Travnikov and Ilyin, 2009;. The model simulates atmospheric transport, chemical transformations, and deposition of three Hg species (GEM, GOM, and PBM).…”

Section: Glemos (Global Emep Multi-media Modeling System)mentioning

confidence: 99%

“…The dry deposition scheme is based on the resistance analogy approach (Wesely and Hicks, 2000). Prescribed fluxes of natural and secondary emissions of Hg from soil and seawater were generated depending on Hg concentrations in soil, soil temperature, and solar radiation for emissions from land and proportional to the primary production of organic carbon in seawater for emissions from the ocean (Travnikov and Ilyin, 2009). In addition, an empirical parameterization of the prompt Hg re-emission from snow-and icecovered surfaces is applied based on observational data.…”

Section: Glemos (Global Emep Multi-media Modeling System)mentioning

confidence: 99%

“…Additionally, emissions from the North and Baltic seas were estimated based on Bieser and Schrum (2016). Boundary conditions were obtained from the GLEMOS model for GEM, GOM, and PBM (Travnikov and Ilyin, 2009) and from TM-5 for all other species (Huijnen et al, 2010). The annual total emissions are based on AMAP for mercury (AMAP, 2013a, b) and EMEP for other species and were speciated and disaggregated to an hourly resolution with the SMOKE for Europe emission model (Bieser et al, 2011a).…”

Section: Cclm-cmaqmentioning

confidence: 99%

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Multi-model study of mercury dispersion in the atmosphere: vertical and interhemispheric distribution of mercury species

et al. 2017

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Abstract. Atmospheric chemistry and transport of mercury play a key role in the global mercury cycle. However, there are still considerable knowledge gaps concerning the fate of mercury in the atmosphere. This is the second part of a model intercomparison study investigating the impact of atmospheric chemistry and emissions on mercury in the atmosphere. While the first study focused on ground-based observations of mercury concentration and deposition, here we investigate the vertical and interhemispheric distribution and speciation of mercury from the planetary boundary layer to the lower stratosphere. So far, there have been few model studies investigating the vertical distribution of mercury, mostly focusing on single aircraft campaigns. Here, we present a first comprehensive analysis based on various aircraft observations in Europe, North America, and on intercontinental flights.The investigated models proved to be able to reproduce the distribution of total and elemental mercury concentrations in the troposphere including interhemispheric trends. One key aspect of the study is the investigation of mercury oxidation in the troposphere. We found that different chemistry schemes were better at reproducing observed oxidized mercury patterns depending on altitude. High concentrations of oxidized mercury in the upper troposphere could be reproduced with oxidation by bromine while elevated concentrations in the lower troposphere were better reproduced by OH and ozone chemistry. However, the results were not always conclusive as the physical and chemical parameterizations in the chemistry transport models also proved to have a substantial impact on model results.

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“…Previous work assumed gas-phase OH and ozone to be the dominant Hg 0 oxidants (Bergan and Rodhe, 2001;Dastoor and Larocque, 2004;Selin et al, 2007;Bullock et al, 2008;Travnikov and Ilyin, 2009;De Simone et al, 2014;Gencarelli et al, 2014). It is now well established that the corresponding HgOH and HgO products are too thermally unstable to enable oxidation to Hg II under atmospheric conditions Goodsite et al, 2004;Calvert and Lindberg, 2005;Hynes et al, 2009;Jones et al, 2016).…”

Section: Introductionmentioning

confidence: 99%

A new mechanism for atmospheric mercury redox chemistry: implications for the global mercury budget

et al. 2017

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Abstract. Mercury (Hg) is emitted to the atmosphere mainly as volatile elemental Hg 0 . Oxidation to water-soluble Hg II plays a major role in Hg deposition to ecosystems. Here, we implement a new mechanism for atmospheric Hg 0 / Hg II redox chemistry in the GEOS-Chem global model and examine the implications for the global atmospheric Hg budget and deposition patterns. Our simulation includes a new coupling of GEOS-Chem to an ocean general circulation model (MITgcm), enabling a global 3-D representation of atmosphereocean Hg 0 / Hg II cycling. We find that atomic bromine (Br) of marine organobromine origin is the main atmospheric Hg 0 oxidant and that second-stage HgBr oxidation is mainly by the NO 2 and HO 2 radicals. The resulting chemical lifetime of tropospheric Hg 0 against oxidation is 2.7 months, shorter than in previous models. Fast Hg II atmospheric reduction must occur in order to match the ∼ 6-month lifetime of Hg against deposition implied by the observed atmospheric variability of total gaseous mercury (TGM ≡ Hg 0 + Hg II (g)). We implement this reduction in GEOS-Chem as photolysis of aqueous-phase Hg II -organic complexes in aerosols and clouds, resulting in a TGM lifetime of 5.2 months against deposition and matching both mean observed TGM and its variability. Model sensitivity analysis shows that the interhemispheric gradient of TGM, previously used to infer a longer Hg lifetime against deposition, is misleading because Southern Hemisphere Hg mainly originates from oceanic emissions rather than transport from the Northern Hemisphere.The model reproduces the observed seasonal TGM variation at northern midlatitudes (maximum in February, minimum in September) driven by chemistry and oceanic evasion, but it does not reproduce the lack of seasonality observed at southern hemispheric marine sites. Aircraft observations in the lowermost stratosphere show a strong TGM-ozone relationship indicative of fast Hg 0 oxidation, but we show that this relationship provides only a weak test of Hg chemistry because it is also influenced by mixing. The model reproduces observed Hg wet deposition fluxes over North America, Europe, and China with little bias (0-30 %). It reproduces qualitatively the observed maximum in US deposition around the Gulf of Mexico, reflecting a combination of deep convection and availability of NO 2 and HO 2 radicals for second-stage HgBr oxidation. However, the magnitude of this maximum is underestimated. The relatively low observed Hg wet deposition over rural China is attributed to fast Hg II reduction in the presence of high organic aerosol concentrations. We find that 80 % of Hg II deposition is to the global oceans, reflecting the marine origin of Br and low concentrations of organic aerosols for Hg II reduction. Most of that deposition takes place to the tropical oceans due to the availability of HO 2 and NO 2 for second-stage HgBr oxidation.

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The EMEP/MSC-E mercury modeling system

Cited by 54 publications

References 38 publications

Recent Advances in Atmospheric Chemistry of Mercury

Recent Advances in Atmospheric Chemistry of Mercury

Multi-model study of mercury dispersion in the atmosphere: vertical and interhemispheric distribution of mercury species

A new mechanism for atmospheric mercury redox chemistry: implications for the global mercury budget

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