Intercomparison study of atmospheric mercury models: 1. Comparison of models with short-term measurements

Ryaboshapko, A. G.; Bullock, O. Russell; Christensen, J. H.; Cohen, Mark; Dastoor, Ashu; Ilyin, Ilia; Petersen, G.; Syrakov, Dimiter; Artz, Richard S.; Davignon, Didier; Draxler, Roland R.; Munthe, John

doi:10.1016/j.scitotenv.2007.01.072

Cited by 48 publications

(30 citation statements)

References 22 publications

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“…Amos et al (2012) find that GEOS-Chem overestimates both components of RHg, with normalized mean biases of 117 % for RGHg and 18 % for PHg (210 % and 96 %, respectively, without in-plume oxidation). In comparing two weeks of ambient measurements over Europe, Ryaboshapko et al (2007) find that RHg shows the largest model-observation discrepancies. In particular, CMAQ-Hg overestimates RGHg by 15-257 % and PHg by 82-380 % (Ryaboshapko et al, 2007).…”

Section: T Holloway Et Al: An Assessment Of Atmospheric Mercury In mentioning

confidence: 93%

“…In comparing two weeks of ambient measurements over Europe, Ryaboshapko et al (2007) find that RHg shows the largest model-observation discrepancies. In particular, CMAQ-Hg overestimates RGHg by 15-257 % and PHg by 82-380 % (Ryaboshapko et al, 2007). Aircraft measurements over the Eastern US for a 12-day period in June 2000 found that CMAQ-Hg overestimated RGHg near the surface, but underestimated concentrations aloft (Sillman et al, 2007).…”

Section: T Holloway Et Al: An Assessment Of Atmospheric Mercury In mentioning

confidence: 93%

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An assessment of atmospheric mercury in the Community Multiscale Air Quality (CMAQ) model at an urban site and a rural site in the Great Lakes Region of North America

et al. 2012

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Abstract. Quantitative analysis of three atmospheric mercury species -gaseous elemental mercury (Hg 0 ), reactive gaseous mercury (RGHg) and particulate mercury (PHg) -has been limited to date by lack of ambient measurement data as well as by uncertainties in numerical models and emission inventories. This study employs the Community Multiscale Air Quality Model version 4.6 with mercury chemistry (CMAQ-Hg), to examine how local emissions, meteorology, atmospheric chemistry, and deposition affect mercury concentration and deposition the Great Lakes Region (GLR), and two sites in Wisconsin in particular: the rural Devil's Lake site and the urban Milwaukee site. Ambient mercury exhibits significant biases at both sites. Hg 0 is too low in CMAQ-Hg, with the model showing a 6 % low bias at the rural site and 36 % low bias at the urban site. Reactive mercury (RHg = RGHg + PHg) is over-predicted by the model, with annual average biases > 250 %. Performance metrics for RHg are much worse than for mercury wet deposition, ozone (O 3 ), nitrogen dioxide (NO 2 ), or sulfur dioxide (SO 2 ). Sensitivity simulations to isolate background inflow from regional emissions suggests that oxidation of imported Hg 0 dominates model estimates of RHg at the rural study site (91 % of base case value), and contributes 55 % to the RHg at the urban site (local emissions contribute 45 %).

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Section: T Holloway Et Al: An Assessment Of Atmospheric Mercury In mentioning

confidence: 93%

Section: T Holloway Et Al: An Assessment Of Atmospheric Mercury In mentioning

confidence: 93%

An assessment of atmospheric mercury in the Community Multiscale Air Quality (CMAQ) model at an urban site and a rural site in the Great Lakes Region of North America

et al. 2012

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“…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. However, until today, we have not fully understood all parts of the global mercury cycle.…”

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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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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“…In past studies, concentrations of atmospheric mercury simulated by GRAHM have been verified against observations (Ryaboshapko et al, 2007a(Ryaboshapko et al, , 2007bDastoor et al, 2008;Durnford et al, 2010Durnford et al, , 2012. Concentrations estimated by GRAHM are within a factor of two of the observed concentrations.…”

Section: The Modelmentioning

confidence: 56%

How relevant is the deposition of mercury onto snowpacks? – Part 1: A statistical study on the impact of environmental factors

Durnford¹,

Dastoor

Steen

et al. 2012

Atmos. Chem. Phys.

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Abstract.A portion of the highly toxic methylmercury that bioaccumulates in aquatic life is created from mercury entering bodies of water with snowpack meltwater. To determine the importance of meltwater as a source of aquatic mercury, it is necessary to understand the environmental processes that govern the behavior of snowpack-related mercury. In this study we investigate relationships among 5 types of snowpack-related mercury observations and 20 model environmental variables. The observation types are the 24-h fractional loss of mercury from surface snow, and the concentrations of mercury in surface snow, seasonal snowpacks, the snowpack meltwater's ionic pulse, and long-term snowpackrelated records. The model environmental variables include those related to atmospheric mercury, insolation, wind, atmospheric stability, snowpack physical characteristics, atmospheric pressure, and solid precipitation. Bivariate and multiple linear regressions were performed twice for each mercury observation type: once with all observations, and once excluding observations from locations where the snowpack's burden of oxidizing and stabilizing halogens is known or presumed to affect snowpack mercury. Since no observations from long-term snowpack-related records were considered affected by halogens, this group of observations was included with the sets of uninfluenced observations and was not discussed with the complete, original sets of observations. When all observations are included, only 37 % of their variability can be explained, on average, with significance confidence levels averaging 81 %; a separate regression model predicts each mercury observation type. Without the influence of halogens, the regression models are able to explain an average of 79 % of the observations' variability with significance confidence levels averaging 97 %. The snowpackrelated mercury observations are most strongly controlled by the dry and wet depositions of oxidized mercury, and by precipitation. Mercury deposited through wet processes is more strongly retained by snowpacks than mercury deposited through dry processes. Revolatilization of mercury deposited through wet processes may be inhibited through burial by fresh snowfalls and/or by its more central location, compared to that of mercury deposited through dry deposition, within snowpack snow grains. The two depositions of oxidized mercury together explain 84 % of the variability in observed concentrations of mercury in surface snow, 52 % of the variability of observed concentrations of mercury in seasonal snowpacks and their meltwater's ionic pulse, and only 20 % of the variability of observed concentrations of mercury in long-term snowpack-related records; other environmental controls seemingly gain in relevance as time passes. The concentration of mercury in long-term records is apparently primarily affected by latitude; both the primary sources

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Intercomparison study of atmospheric mercury models: 1. Comparison of models with short-term measurements

Cited by 48 publications

References 22 publications

An assessment of atmospheric mercury in the Community Multiscale Air Quality (CMAQ) model at an urban site and a rural site in the Great Lakes Region of North America

An assessment of atmospheric mercury in the Community Multiscale Air Quality (CMAQ) model at an urban site and a rural site in the Great Lakes Region of North America

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

How relevant is the deposition of mercury onto snowpacks? – Part 1: A statistical study on the impact of environmental factors

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