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Gerhard Petersen GKSS Research Centre

4th Meeting of the EMEP Task Force on Measurement and Modelling Valencia, Spain, April 9-11 2003 Recent Developments in Mercury Modelling. Gerhard Petersen GKSS Research Centre Institute for Coastal Research / System Analysis and Modelling Max-Planck-Strasse 1 D-21502 Geesthacht GERMANY.

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Gerhard Petersen GKSS Research Centre

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  1. 4th Meeting of the EMEP Task Force on Measurement and Modelling Valencia, Spain, April 9-11 2003Recent Developments in Mercury Modelling Gerhard Petersen GKSS Research Centre Institute for Coastal Research / System Analysis and Modelling Max-Planck-Strasse 1 D-21502 Geesthacht GERMANY

  2. Background and Motivation for Atmospheric Mercury Modelling in Europe • UN-ECE Convention on Long-Range Transboundary Air Pollution • (Aarhus Protocol on Heavy Metals, June 1998) • EU Air Quality Directive on Mercury • European Marine Environment Protection Conventions • (OSPARCOM, HELCOM) • Arctic Monitoring and Assessment Program • (AMAP)

  3. Main Activities in Atmospheric Mercury Modelling in Europe • EMEP Meteorological Synthesizing Centre-East (EMEP MSC-E), Moscow, Russia, European scale modelling for UN-ECE CLRTAP, HELCOM, mercury model intercomparison study. • Institute for Atmospheric Pollution - National Research Council (IIA-CNR), Rende, Italy, European scale modelling focusing on the Mediterrenean area, EU Air Quality Directive on Mercury. • GKSS Research Center Geesthacht, • Hamburg, Germany, European scale modelling for EU focusing on the North Sea and the Baltic Sea, • scientific support for EMEP MSC-E. • National Environmental Research Centre (NERI), • Risö, Denmark, hemispheric scale modelling for the Arctic.

  4. Priority Metals of Concern and their Typical Concentrations in Ambient Air over Europe lead 5 - 50 ng m-3 cadmium 0.05-0.5 ng m-3 mercury TGM (Hg0) 1 - 4 ng m-3 RGM (HgCl2) 0.005 - 0.05 ng m-3 TPM (Hg(part.)) 0.01 - 0.1 ng m-3 MeHg 0.0005 - 0.01 ng m-3

  5. ADOM - main features (1)model domain • 3-d Eulerian grid model • with a time step of • 1 hour • rotated spherical • coordinate system • of the HIgh Resolution • Limited Area Weather • Prediction Model • (HIRLAM) with 76 by 76 • grid cells • ~55x55 km2 grid cell size • 12 vertical layers between • 1 and 10 000 m with 8 • layers below 2000 m

  6. ADOM-Main Features (5)Atmospheric Mercury Chemistry Scheme 21 reactions among 14 species based on the Chemistry of Atmospheric Mercury (CAM) model of the Swedish Environmental Research Institute (IVL) G(1) - G(4) mercury species in ambient air AQ(1) - AQ(10) mercury species in the aqueous phase R1 - R5 mass transfer rate expressions R6 - R 17 aqueous phase reaction rate expressions R18 - R19 equilibrium rate expressions for adsorption R20 - R21 gas phase rection rate expressions chemical solver using the Young and Boris predictor-corrector scheme

  7. Hg Physical Chemistry System for the Community Multi-Scale Air Quality (CMAQ) Model (adopted from Bullock and Brehme, 2002) Hg2+ sorbed to Carbon Aerosol RGM as HgCl2(g) Particulate Hg HgOHCl HgCl2(aq) Cl- Hg(SO3)22- Cl- HgOH+ Hg2+ SO32- SO32- OH- OH- HgSO3 HO2 Hg(OH)2 O3, OH, HOCl/ OCl- decomp. h . v Hg0(g) Hg0(aq)

  8. Mercury Emissions in Europe units: tonnes per year 1990 463 tonnes per year 1995 327 tonnes per year

  9. Mercury Emissions in Europe (3) Mercury Emission Inventory for 1995 (Norwegian Institute for Air Research NILU, 2000) Hg0 205 t y-1 HgCl2 96 t y-1 Hg(part.) 26 t y-1 TOTAL 327 t y-1

  10. ADOM Results (1) monthly average concentration of Hg0 in ambient air November 1998 units: ng m-3 < 1.3 1.3 - 1.4 1.4 - 1.5 1.5 - 1.6 1.6 - 1.7 > 1.7

  11. ADOM Results (2) monthly average concentration of HgCl2 in ambient air November 1998 units: pg m-3 < 20 20 - 25 25 - 30 30 - 35 35 - 40 > 40

  12. ADOM Results (3) monthly average concentration of Hg(part.) in ambient air November 1998 units: pg m-3 < 20 20 - 25 25 - 30 30 - 35 35 - 40 > 40

  13. monthly dry deposition flux of Hg November 1998 units: ng m-2 month-1 < 100 100 - 250 250 - 500 500 - 750 750 - 1000 > 1000 ADOM Results (4)

  14. monthly wet deposition flux of Hg November 1998 units: ng m-2 month-1 < 100 100 - 250 250 - 500 500 - 750 750 - 1000 > 1000 ADOM results (5)

  15. Location of four Monitoring Sites in Germany and Swedenfor Model Validation Aspvreten Roervik Zingst Neuglobsow mercury emission rates units: tonnes per year

  16. Comparison of Observed and Model Predicted Total Gaseous Mercury (TGM) Concentrations in Air November / December 1998 ZINGST Observation November/ December 1998 Model prediction 1990 emissions NEUGLOBSOW Model prediction 1995 emissions

  17. Comparison of Observed and Model Predicted Reactive Gaseous Mercury (RGM) Concentrations in Air November 1999 (adopted from MSC-E) Neuglobsow (Germany) Mace Head (Ireland)

  18. Comparison of Observed and Model Predicted Total Particulate Mercury (TPM) Concentrations in Air November 1999 Neuglobsow Zingst Rörvik Aspvreten

  19. Observed and Calculated Average Mercury Concentration in Precipitation at four Baltic Sea Coastal Sites February-March 1998 (a) Kap Arkona D (b) Hel PL (c) Preila LT (d) Hoburg S

  20. Summary and Conclusions (1) • Main Progress: • Three comprehensive European scale Eulerian model systems for atmospheric mercury species incorporating state-of-science mercury chemistry schemes are available now for UN-ECE LRTAP, OSPARCOM, HELCOM and EU Air Quality Directive purposes: • - the MSC-E model of the EMEP Meteorological Synthesizing Center East (Russia) • - the MAMCS model system of the IIA-CNR (Italy) • - the ADOM model system for mercury of GKSS (Germany) • Development of a Northern hemisphere model is underway now at NERI (Denmark) • First versions of speciated emission inventories for mercury species (Hg0, Hg(II) and Hg(part.)) have been compiled by NILU (Norway) and are used now for model calculations • A model intercomparison study organized by EMEP MSC-E is underway now under participation of European models and models from the U.S. and Canada.

  21. Summary and Conclusions (2) • Main Problems: • European emission inventories have to be updated for 1996 and following years. Their improvement with respect to mercury speciation (e. g. flue gas measurementsof the most important source categories) is absolutely necessary. • Air / Surface fluxesof gaseous mercury species as a function of meterological and geophysical parameters have to be measured including potential re-emissions from areas of former high deposition fluxes in Central Europe. • More field measurements of mercury species (RGM, TPM) are needed for model validation purposes. • Mercury chemistry schemes have to be improved with respect to observed RGM formation over sea areas and adsorption of mercury species on particles (soot). • For European scale models, time dependent vertical profiles of Hg0 concentrations at model inflow boundaries calculated by hemispheric or global scale models have to be introduced. There is evidence now that contributions from the global background to areas in Europe can be significant (e.g. about 40% for the Baltic Sea).

  22. Comparison of Observed and Model Predicted Reactive Gaseous Mercury (RGM) Concentrations in Air November 1999 Neuglobsow Rörvik Aspvreten

  23. Temporal Trend of Mercury Concentrations in Ambient Air in the Northern Hemisphere 1977-2001

  24. ADOM-Main Features (3)Relationship between ADOM modules and input parameters Input Data Pollutant Transport Model ADOM Meteorological Pre-Processor emission data base EUROPE: HIRLAM High Resolution Limited Area Weather Prediction Model transport and diffusion geophysical data dry deposition upper and surface meteorology gas-phase chemistry NORTH AMERICA: CMC Canadian Meteorological Center Large Scale Model initial conditions wet scavenging boundary conditions aqueous phase chemistry cloud physics secondary pollutants

  25. ADOM Main Features (4)Parameterization of the life cycle of a cumulus cloud z air pollutants ingested into clouds cloud top formation of clouds side air outflow up and down motion of air parcels chemical reactions in liquid water side air inflow dwell phase x cloud base air pollutants ejected from dissipating clouds below cloud air inflow precipitation precipitation dissipation of clouds y

  26. Major Pathways Governing Hg Chemistry in the Atmosphere (adopted from Ryaboshapko et al., 2002) oxidation Hg0 Hg(II) Hg(p) gas phase oxidation dissolution Hg0 Hg(II) Hg(p) aqueous phase reduction adsorption to soot Hg(p)

  27. annual atmospheric input rates of mercury to the Baltic Sea

  28. Transboundary Fluxes of Mercury in Europe 1998 source: EMEP MSC-East, Moscow exported from Germany to

  29. Transboundary Fluxes of Mercury in Europe 1998 source: EMEP MSC-E, Moscow imported to Germany from undefined origin (global background) 7447 kg/year 41 % Germany 8105 kg/year 46 %

  30. total (dry and wet) monthly flux of mercury to the Baltic Sea area February 1998 units: ng m-2 month-1 < 800 800-1000 1000-1200 1200-1500 1500-2000 > 2000 ADOM results (4)

  31. model predicted atmospheric input of mercury into the Baltic Sea (from EU MAST III Baltic Sea System Study BASYS, Subproject 5 Atmospheric Load) monthly and annual input rates from anthropogenic emissions in Europe and global background monthly and annual input rates from global background only

  32. annual emission rates and main source categories for heavy metals in Europe 1980 and 1990 LEAD 1980: 89 000 tons 1990: 40 400 tons CADMIUM 1980: 1 100 tons 1990: 610 tons MERCURY 1980: 730 tons 1990: 460 tons 75% 70% 65% 55% 55% 50% 35% 35% 25% 18% 15% 14% 9% 4% 3% 5% 2% 1% waste- incineration road- transort industrial production waste- incineration public power district heating industrial & residential combustion waste- incineration public power district heating industrial & residential combustion public power district heating industrial & residential combustion production processes industrial production

  33. Mercury Emissions in Europe (2) Mercury Emission Inventory for 1990 (Umweltbundesamt, 1994) Hg0 417 t y-1 HgCl2 23 t y-1 Hg(part.) 23 t y-1 TOTAL 463 t y-1

  34. Quecksilberemissionen in Europa

  35. ADOM results monthly precipitation amount November 1998 units: mm per month < 30 30-90 90-150 150-210 219-270 > 270

  36. Major Pathways Governing Hg Chemistry in the Atmosphere (adopted from Ryaboshapko et al., 2002) oxidation Hg0 Hg(II) Hg(p) gas phase oxidation dissolution Hg0 Hg(II) Hg(p) aqueous phase reduction adsorption to soot Hg(p)

  37. 416.3 10 000.0 layer 4 layer 12 z [m] 250.7 6894.5 Z [m] layer 3 layer 11 135.8 4741.6 layer 10 layer 2 3249.2 56.2 layer 9 2214.5 layer 8 1497.2 layer 1 656.3 layer 6 layer 5 production processes industrial and residential combustion waste incineration district heating public power layer 1-4 ADOM main features (2)vertical grid and emission height 1000.0 layer 7 416.3

  38. Comparison of Observed and Model Predicted Reactive Gaseous Mercury (RGM) Concentrations in Air November 1999 Neuglobsow Rörvik Aspvreten

  39. Temporal Trend of Mercury Concentrations in Ambient Air in the Northern Hemisphere 1977-2001

  40. ADOM-Main Features (3)Relationship between ADOM modules and input parameters Input Data Pollutant Transport Model ADOM Meteorological Pre-Processor emission data base EUROPE: HIRLAM High Resolution Limited Area Weather Prediction Model transport and diffusion geophysical data dry deposition upper and surface meteorology gas-phase chemistry NORTH AMERICA: CMC Canadian Meteorological Center Large Scale Model initial conditions wet scavenging boundary conditions aqueous phase chemistry cloud physics secondary pollutants

  41. ADOM Main Features (4)Parameterization of the life cycle of a cumulus cloud z air pollutants ingested into clouds cloud top formation of clouds side air outflow up and down motion of air parcels chemical reactions in liquid water side air inflow dwell phase x cloud base air pollutants ejected from dissipating clouds below cloud air inflow precipitation precipitation dissipation of clouds y

  42. annual atmospheric input rates of mercury to the Baltic Sea

  43. Transboundary Fluxes of Mercury in Europe 1998 source: EMEP MSC-East, Moscow exported from Germany to

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