Journal cover Journal topic
Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
doi:10.5194/acp-2016-924
© Author(s) 2016. This work is distributed
under the Creative Commons Attribution 3.0 License.
Research article
31 Oct 2016
Review status
A revision of this discussion paper was accepted for the journal Atmospheric Chemistry and Physics (ACP) and is expected to appear here in due course.
Multi-model study of mercury dispersion in the atmosphere: Atmospheric processes and model evaluation
Oleg Travnikov1, Hélène Angot2, Paulo Artaxo3, Mariantonia Bencardino4, Johannes Bieser5, Francesco D’Amore4, Ashu Dastoor6, Francesco De Simone4, María del Carmen Diéguez7, Aurélien Dommergue2,8, Ralf Ebinghaus5, Xin Bin Feng9, Christian N. Gencarelli4, Ian M. Hedgecock4, Olivier Magand8, Lynwill Martin10, Volker Matthias5, Nikolay Mashyanov11, Nicola Pirrone12, Ramesh Ramachandran13, Katie Alana Read14, Andrei Ryjkov6, Noelle E. Selin15,16, Fabrizio Sena17, Shaojie Song15, Francesca Sprovieri4, Dennis Wip18, Ingvar Wängberg19, and Xin Yang20 1Meteorological Synthesizing Centre – East of EMEP, Moscow, Russia
2University Grenoble Alpes, Laboratoire de Glaciologie et Géophysique de l’Environnement, Grenoble, France
3University of Sao Paulo, Sao Paulo, Brazil
4CNR Institute of Atmospheric Pollution Research, Rende, Italy
5Institute of Coastal Research, Helmholtz-Zentrum Geesthacht, Geesthacht, Germany
6Air Quality Research Division, Environment and Climate Change Canada, Canada
7INIBIOMA-CONICET-UNComa, Bariloche, Argentina
8CNRS, Laboratoire de Glaciologie et Géophysique de l’Environnement, Grenoble, France
9Institute of Geochemistry, State Key Laboratory of Environmental Geochemistry, Chinese Academy of Sciences, Guiyang, China
10Cape Point GAW Station, Climate and Environment Research & Monitoring, South African Weather Service, Stellenbosch, South Africa
11St. Petersburg State University, St. Petersburg, Russia
12CNR Institute of Atmospheric Pollution Research, Rome, Italy
13Institute for Ocean Management, Anna University, Chennai, India
14NCAS, University of York, York, UK
15Department of Earth, Atmospheric and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA, USA
16Institute for Data, Systems, and Society, Massachusetts Institute of Technology, Cambridge, MA, USA
17Joint Research Centre, Ispra, Italy
18Department of Physics, University of Suriname, Paramaribo, Suriname
19IVL, Swedish Environmental Research Inst. Ltd., Göteborg, Sweden
20British Antarctic Survey, Cambridge, UK
Abstract. Current understanding of mercury (Hg) behaviour in the atmosphere contains significant gaps. Some key characteristics of Hg processes including anthropogenic and geogenic emissions, atmospheric chemistry, and air-surface exchange are still poorly known. This study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data from ground-based sites and simulation results of chemical transport models. A variety of long-term measurements of gaseous elemental Hg (GEM) and reactive Hg (RM) concentration as well as Hg wet deposition flux has been compiled from different global and regional monitoring networks. Four contemporary global-scale transport models for Hg were applied both in their state-of-the-art configurations and for a number of numerical experiments aimed at evaluation of particular processes. Results of the model simulation were evaluated against measurements. As it follows from the analysis the inter-hemispheric gradient of GEM is largely formed by the spatial distribution of anthropogenic emissions which prevail in the Northern Hemisphere. Contribution of natural and secondary emissions enhances the south-to-north gradient but their effect is less significant. The atmospheric chemistry does not affect considerably both spatial distribution and temporal variation of GEM concentration in the surface air. On the other hand, RM air concentration and wet deposition are largely defined by oxidation chemistry. The Br oxidation mechanism allows successfully reproducing observed seasonal variation of the RM / GEM ratio in the near-surface layer, whereas it predicts maximum in wet deposition in spring instead of summer as observed at monitoring sites located in North America and Europe. Model runs with the OH chemistry correctly simulate both the periods of maximum and minimum values and the amplitude of observed seasonal variation but lead to shifting the maximum RM / GEM ratios from spring to summer. The O3 chemistry does not provide significant seasonal variation of Hg oxidation. Thus, performance of the considered Hg oxidation mechanisms differs in reproduction of different observed parameters that can imply possibility of more complex chemistry and multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.

Citation: Travnikov, O., Angot, H., Artaxo, P., Bencardino, M., Bieser, J., D’Amore, F., Dastoor, A., De Simone, F., Diéguez, M. D. C., Dommergue, A., Ebinghaus, R., Feng, X. B., Gencarelli, C. N., Hedgecock, I. M., Magand, O., Martin, L., Matthias, V., Mashyanov, N., Pirrone, N., Ramachandran, R., Read, K. A., Ryjkov, A., Selin, N. E., Sena, F., Song, S., Sprovieri, F., Wip, D., Wängberg, I., and Yang, X.: Multi-model study of mercury dispersion in the atmosphere: Atmospheric processes and model evaluation, Atmos. Chem. Phys. Discuss., doi:10.5194/acp-2016-924, in review, 2016.
Oleg Travnikov et al.
Interactive discussionStatus: closed
AC: Author comment | RC: Referee comment | SC: Short comment | EC: Editor comment
Printer-friendly Version - Printer-friendly version      Supplement - Supplement
 
RC1: 'Accept with English polishing', Anonymous Referee #1, 16 Dec 2016 Printer-friendly Version 
AC1: 'Reply to comments by Referee #1', Oleg Travnikov, 03 Mar 2017 Printer-friendly Version 
 
RC2: 'Referee Comment', Anonymous Referee #2, 27 Dec 2016 Printer-friendly Version 
AC2: 'Reply to comments by Referee #2', Oleg Travnikov, 03 Mar 2017 Printer-friendly Version 
Oleg Travnikov et al.
Oleg Travnikov et al.

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Short summary
The study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data and simulation results of chemical transport models. Evaluation of the model simulations and numerical experiments against observations allows explaining spatial and temporal variations of Hg concentration in the near-surface layer and shows possibility of multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.
The study provides a complex analysis of processes governing Hg fate in the atmosphere involving...
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