Multiscale modeling of the atmospheric fate and transport of mercury

Seigneur, Christian; Karamchandani, Prakash; Lohman, Kristen; Vijayaraghavan, Krish; Shia, Run‐Lie

doi:10.1029/2000jd000273

Cited by 133 publications

(104 citation statements)

References 45 publications

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“…The major chemical mechanisms in the gas phase include Hg oxidation by O 3 and OH radicals with reaction rate constants taken from Hall (1995) and Sommar et al (2001), respectively. The latter was scaled down by a factor of 0.1 within and below clouds to account for reduced photochemical activity (Seigneur et al, 2001). The O 3 and OH concentration fields are imported from MOZART (Emmons et al, 2010).…”

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

confidence: 99%

“…In the last decades, general chemistry transport models (CTMs) have been extended to model the global mercury cycle by including mercury chemistry and partitioning (Bergan et al, 1999;Xu et al, 2000;Lee et al, 2001;Petersen et al, 2001;Seigneur et al, 2001;Dastoor and Larocque, 2004;Selin et al, 2007;Hedgecock and Pirrone, 2004). Since then, extensive model intercomparison studies have been performed to evaluate and improve the original models (Bullock et al, 2008;Ryaboshapko et al, 2002Ryaboshapko et al, , 2007a.…”

Section: Introductionmentioning

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

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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

et al. 2017

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“…Earlier models of atmospheric Hg included parameterizations for the sorption of dissolved Hg species to soot particles suspended in cloud water (Petersen et al, 1998;Seigneur et al, 2001;Bullock and Brehme, 2002;Dastoor and Larocque, 2004) based on experimental results from Petersen et al (1995) and Seigneur et al (1998). In more recent years, models of atmospheric Hg have taken various approaches to treating Hg(II) gas-particle partitioning.…”

mentioning

confidence: 99%

Gas-particle partitioning of atmospheric Hg(II) and its effect on global mercury deposition

Amos

Jacob²,

Holmes³

et al. 2012

Atmos. Chem. Phys.

412

459

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Abstract. Atmospheric deposition of Hg(II) represents a major input of mercury to surface environments. The phase of Hg(II) (gas or particle) has important implications for deposition. We use long-term observations of reactive gaseous mercury (RGM, the gaseous component of Hg(II)), particle-bound mercury (PBM, the particulate component of Hg(II)), fine particulate matter (PM 2.5 ), and temperature (T ) at five sites in North America to derive an empirical gas-particle partitioning relationship log 10 (K −1 ) = (10±1)-(2500±300)/T where K = (PBM/PM 2.5 )/RGM with PBM and RGM in common mixing ratio units, PM 2.5 in µg m −3 , and T in K. This relationship is within the range of previous work but is based on far more extensive data from multiple sites. We implement this empirical relationship in the GEOS-Chem global 3-D Hg model to partition Hg(II) between the gas and particle phases. The resulting gas-phase fraction of Hg(II) ranges from over 90 % in warm air with little aerosol to less than 10 % in cold air with high aerosol. Hg deposition to high latitudes increases because of more efficient scavenging of particulate Hg(II) by precipitating snow. Model comparison to Hg observations at the North American surface sites suggests that subsidence from the free troposphere (warm air, low aerosol) is a major factor driving the seasonality of RGM, while elevated PBM is mostly associated with high aerosol loads. Simulation of RGM and PBM at these sites is improved by including fast in-plume reduction of Hg(II) emitted from coal combustion and by assuming that anthropogenic particulate Hg(p) behaves as semivolatile Hg(II) rather than as a refractory particulate component. We improve the simulation of Hg wet deposition fluxes in the US relative to a previous version of GEOS-Chem; this largely reflects independent improvement of the washout algorithm. The observed wintertime minimum in wet deposition fluxes is attributed to inefficient snow scavenging of gas-phase Hg(II).

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“…Developing economies and increased energy needs have resulted in a transfer of dominant global emissions of atmospheric mercury from North America/Europe to Asia (Pacyna et al 2006;Seigneur et al 2001). Led by China, Asian sources emitted approximately 54% of the global total in 2000 (Wu et al 2006).…”

Section: Asian Mercury Sourcesmentioning

confidence: 99%

Mercury Sources to Lake Ozette and Lake Dickey: Highly Contaminated Remote Coastal Lakes, Washington State, USA

Furl

Colman

Bothner

2009

Water Air Soil Pollut

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Mercury concentrations in largemouth bass and mercury accumulation rates in age-dated sediment cores were examined at Lake Ozette and Lake Dickey in Washington State. Goals of the study were to compare concentrations in fish tissues at the two lakes with lakes in a larger statewide dataset and evaluate factors influencing lake loading at Ozette and Dickey, which may include: catchment disturbances, coastal mercury cycling, and the role of trans-Pacific Asian mercury. Mercury fish tissue concentrations at the lakes were among the highest recorded in Washington State. Wet deposition and historical atmospheric monitoring from the area show no indication of enhanced deposition from Asian sources or coastal atmospheric processes. Sediment core records from the lakes displayed rapidly increasing sedimentation rates coinciding with commercial logging. The unusually high mercury flux rates and mercury tissue concentrations recorded at Lake Ozette and Lake Dickey appear to be associated with logging within the catchments.

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Multiscale modeling of the atmospheric fate and transport of mercury

Cited by 133 publications

References 45 publications

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

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

Gas-particle partitioning of atmospheric Hg(II) and its effect on global mercury deposition

Mercury Sources to Lake Ozette and Lake Dickey: Highly Contaminated Remote Coastal Lakes, Washington State, USA

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