Sensitivity model study of regional mercury dispersion in the atmosphere

Gencarelli, Christian N.; Carbone, Francesco; Simone, Francesco De; Hedgecock, Ian M.; Matthias, Volker; Travnikov, Oleg; Yang, Xin; Pirrone, Nicola

doi:10.5194/acp-17-627-2017

Cited by 21 publications

(20 citation statements)

References 72 publications

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“…It can be seen that the models generally underestimate mercury concentrations. This is in line with many previous model studies which found that models tend to underestimate current TM concentrations in Europe (Bieser et al, 2014b;Chen et al, 2014;Muntean et al, 2014;Gencarelli et al, 2017). Based on a model run from 1996 to 2008, Muntean et al (2014) hypothesized that this was due to an overestimation of emission reductions in the last decade.…”

Section: Europesupporting

confidence: 87%

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: Europesupporting

confidence: 87%

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

et al. 2017

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“…Gencarelli et al [68] simulated the deposition, transport and chemical interactions of atmospheric Hg over Europe for the year of 2013. The outputs of 14 model sensitivity tests were compared with field data from 28 monitoring sites.…”

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

confidence: 99%

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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“…Atmospheric redox chemistry of Hg plays an important role in understanding Hg transport and deposition in the atmosphere. However, mechanisms of Hg oxidation in the atmosphere are not well understood, causing uncertainty in the simulation results of Hg chemical transport models (Ariya et al, ; Gencarelli et al, ; Pacyna et al, ; Travnikov et al, ; L. M. Zhang et al, ). Observational evidence exists that the Br‐mediated oxidation pathway plays a dominant role in GEM oxidation in certain atmospheric environments (e.g., the marine boundary, polar regions, and the upper troposphere; Ariya et al, ; Gratz et al, ; Holmes et al, ; Horowitz et al, ).…”

Section: Methodsmentioning

confidence: 99%

“…However, limited observational data exist with respect to this mechanism and Br concentration in the global atmosphere (Kos et al, ; Travnikov et al, ). On the other hand, despite questions regarding viability and significance of GEM oxidation mechanisms involving in O 3 and OH (Gratz et al, ; Holmes et al, ; Horowitz et al, ), both theoretical and laboratory studies suggest that these mechanisms can exist in the atmosphere in the presence of aerosol and secondary reactions (Ariya et al, ; Feinberg et al, ; Gencarelli et al, ; Si & Ariya, ; Subir et al, ; Travnikov et al, ). Under polluted conditions in urban areas of China, Hong et al () suggests that the O 3 /OH oxidation pathway dominates GOM formation and that such pathway can be enhanced in the presence of NO 2 .…”

Section: Methodsmentioning

confidence: 99%

Assessment of Regional Mercury Deposition and Emission Outflow in Mainland China

et al. 2018

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Mainland China is the largest emission region of anthropogenic mercury (Hg) in the world. There have been concerns regarding the emission outflow and chemical transport budget of Hg in the region. Earlier assessments of Hg chemical transport were based on relatively outdated emission data. Recent estimates for anthropogenic (Wu et al., 2016, https://doi.org/10.1021/acs.est.6b04308) and natural Hg emissions (X. Wang, Lin, et al., 2016, https://doi.org/10.5194/acp-16-11125-2016) show substantial differences from earlier emission inventories. In this study, we applied the updated Hg emission estimates to reassess the regional transport budget using Community Multiscale Air Quality‐Hg v5.1. Our results show that the variation of simulated concentration, deposition, and associated emission outflow of Hg are primarily influenced by the spatial‐temporal variation of Hg emissions, monsoon shifts, and particulate matter pollution in China. Total Hg deposition in Mainland China is estimated to be 422 Mg/year, and approximately two thirds of the deposition is contributed by domestic emissions. The net Hg transport budget from Mainland China is 511 Mg/year, contributing to 10% of Hg deposition in other regions of the world. This reassessment points to a ~25% reduction in total annual outflow compared to the previous estimate by Lin et al. (2010, https://doi.org/10.5194/acp-10-1853-2010). Such reduction is mainly caused by changes in Hg emission quantity, speciation, and spatial/temporal distributions. More modeling studies focusing on reducing uncertainties of emission inventories and Hg atmospheric chemistry are needed for continuous assessment of Hg emission outflow in this emission‐intensive region.

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Sensitivity model study of regional mercury dispersion in the atmosphere

Cited by 21 publications

References 72 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

Recent Advances in Atmospheric Chemistry of Mercury

Assessment of Regional Mercury Deposition and Emission Outflow in Mainland China

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