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Volume 16, issue 13
Atmos. Chem. Phys., 16, 8461–8478, 2016
https://doi.org/10.5194/acp-16-8461-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.

Special issue: Data collection, analysis and application of speciated atmospheric...

Atmos. Chem. Phys., 16, 8461–8478, 2016
https://doi.org/10.5194/acp-16-8461-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 12 Jul 2016

Research article | 12 Jul 2016

Investigation of processes controlling summertime gaseous elemental mercury oxidation at midlatitudinal marine, coastal, and inland sites

Zhuyun Ye1, Huiting Mao1, Che-Jen Lin2,3, and Su Youn Kim4 Zhuyun Ye et al.
  • 1Department of Chemistry, State University of New York, College of Environmental Science and Forestry, Syracuse, NY 13210, USA
  • 2Center for Advances in Water and Air Quality, Lamar University, Beaumont, TX 77710, USA
  • 3Department of Civil and Environmental Engineering, Lamar University, Beaumont, TX 77710, USA
  • 4R&D Program Evaluation Division Office of National Evaluation and Analysis Korea Institute of S&T Evaluation and Planning (KISTEP), Seoul, South Korea

Abstract. A box model incorporating a state-of-the-art chemical mechanism for atmospheric mercury (Hg) cycling was developed to investigate the oxidation of gaseous elemental mercury (GEM) at three locations in the northeastern United States: Appledore Island (AI; marine), Thompson Farm (TF; coastal, rural), and Pack Monadnock (PM; inland, rural, elevated). The chemical mechanism in this box model included the most up-to-date Hg and halogen chemistry. As a result, the box model was able to simulate reasonably the observed diurnal cycles of gaseous oxidized mercury (GOM) and chemical speciation bearing distinct differences between the three sites. In agreement with observations, simulated GOM diurnal cycles at AI and TF showed significant daytime peaks in the afternoon and nighttime minimums compared to flat GOM diurnal cycles at PM. Moreover, significant differences in the magnitude of GOM diurnal amplitude (AI > TF > PM) were captured in modeled results. At the coastal and inland sites, GEM oxidation was predominated by O3 and OH, contributing 80–99 % of total GOM production during daytime. H2O2-initiated GEM oxidation was significant (∼ 33 % of the total GOM) at the inland site during nighttime. In the marine boundary layer (MBL) atmosphere, Br and BrO became dominant GEM oxidants, with mixing ratios reaching 0.1 and 1 pptv, respectively, and contributing ∼ 70 % of the total GOM production during midday, while O3 dominated GEM oxidation (50–90 % of GOM production) over the remaining day when Br and BrO mixing ratios were diminished. The majority of HgBr produced from GEM+Br was oxidized by NO2 and HO2 to form brominated GOM species. Relative humidity and products of the CH3O2+BrO reaction possibly significantly affected the mixing ratios of Br or BrO radicals and subsequently GOM formation. Gas–particle partitioning could potentially be important in the production of GOM as well as Br and BrO at the marine site.

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In this study, a state-of-the-art chemical mechanism was incorporated into a box model to investigate the atmospheric Hg cycling in different environments. As a result, for each of the three environments, GOM diurnal cycles of over half the selected cases were reasonably represented by the box model. A realistic model can be a powerful tool, providing important information on atmospheric Hg cycling and implications for policy makers.
In this study, a state-of-the-art chemical mechanism was incorporated into a box model to...
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