Modeling trans-boundary transport of benzo(a)pyrene over Europe with CMAQ A. Aulinger, V. Matthias, M. Quante, Institute for Coastal Research GKSS Research Center Geesthacht, Germany

Outline Introduction: Why PAHs ? Model modification and set up Emissions Model results Comparison with measurements Conclusions and outlook

Why PAHs ? PAHs imperil humans and ecosystems highly bioaccumulative (food chain) persistent in various environmental compartments significant adverse effects already at low doses carcinogenic impair immune system impair reproduction B(a)P Object of international reduction conventions (Target values for air concentrations - EU: 1 ng/m3 (annual average), UK: 0.25 ng/m3) Emissions are likely to increase wood burning, ship traffic

MM5 and CMAQ for annual simulations model domain 30 vertical layers up to 100 hPa 54x54 km2 grid 18x18 km2 grid

Model set up for annual simulations CMAQ: Version 4.5 CB IV chemistry scheme Aero 4 module incl. SOA formation Anthrop. emissions from IER Stuttgart based on EMEP and EPER data base Natural emissions from GEIA and RETRO database B(a)P emissions from Denier van der Gon et al. (TNO report, 2005)

Some chemical species in CMAQ (CB-IV mechanism): Aerosols in three size classes (visibility also calculated) 7 inorganic, 2 organic nitrogen species SO2, sulfate (sulfuric acid) Seasalt Anthropogenic and biogenic volatile organics O3, H2O2, OH Benzo(a)pyrene

Partitioning

Electricity generation Iron and steel production Emissions major sources Residential heating Road transport Electricity generation Iron and steel production Incineration of household waste Ship engines Oil platforms Wildfires B(a)P emissions in 2000 PAHs are formed by any incomplete combustion of organic matter

Emissions Time scheme Constant (case a) Seasonality after TNO (case b)

Emissions Temperature dependence

Emissions

Emissions

Time variant emissions (expl. Berlin 2000) case c

Simulations vs. measurements

Simulations vs. measurements

Correlations Station Roervik, SE, rural, monthly means 0.479 0.636 Case A Case B Case C Roervik, SE, rural, monthly means 0.479 0.636 0.689 Aspvreten, SE, rural, monthly means -0.105 0.239 0.183 Pallas, FI, remote, monthly means 0.746 0.763 0.595 Preila, LT, urban, monthly means 0.639 0.653 0.798 Kosetice, CZ rural, monthly means 0.845 0.829 0.971 Lista, NO, remote monthly means -0.058 -0.052 -0.09 Bornhoeved, DE, rural, weekly means 0.684 0.724 0.718 Radebeul, DE, suburban 2-day means 0.581 0.646 0.727

Depositions into the Baltic Sea Total depositions in 2000 in t   Depositions in t Case A 12.05 Case B 12.82 Case C 13.43

CMAQ with 12 vertical layers  10-15% lower concentrations CMAQ results: B(a)P concentrations in Europe for lowest layer total annual amount of emitted B(a)P was the same for both model runs (based on 2000 data) CMAQ with 12 vertical layers  10-15% lower concentrations

CMAQ results: B(a)P concentrations over the North Sea for lowest layer

CMAQ results: B(a)P wet deposition over the North Sea

Precipitation

CMAQ results vs. EMEP measurements: B(a)P concentrations statistics CMAQ model results vs. EMEP measurements, statistical quality indicators, times series year 2000 and 2001

Emission data

CMAQ results vs. EMEP measurements: PM10 concentrations stations, daily means 2000 PM10 [gm-3] Deuselbach, Germany, 480 m asl Mean (meas) 14.8 mg/m3 bias -3.4 mg/m3 rms error 7.7 mg/m3 Correlation 0.47 IOA 0.64 measurements model PM10, IOA, total year

Conclusions and outlook Correlations simulations vs. measurements already acceptable with constant emissions but notably better with time-variant emissions Simulations tend to overestimate observations Differences between different simulation periods more prominent concerning deposition than concentrations Best agreement with measurement stations in the vicinity of sources Higher resolved model domain and emissions required, for investigation on small regional scales Long-term studies over several years planned Degradation of pollutants should be considered Ship emissions will be considered We recommend the revision of emission data

Outlook - ship emissions

Thank you for your attention THE END