1. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante Using CMAQ for modelling the polycyclic aromatic hydrocarbon distribution over coastal Europe: Status and prospects M. Quante, A. Aulinger, V. Matthias, I. Bewersdorff Institute for Coastal Research GKSS Research Center Geesthacht, Germany

2. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante GKSS is member of the Helmholtz Association Material Research Polymer Research Coastal Research GKSS Research Center

3. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante  Main objectives  Why PAHs ?  Model modification and set up  Emissions  Model studies and selected results  Comparison with measurements  PAHs from ship traffic  Conclusions and outlook Outline

4. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante Estimation and assessment of depositions and concentration levels of PAHs in coastal ecosystems at long time scales Evaluation of past and forecast of future developments (scenarios) Contribution to „cycle of substances“ in coastal ecosystems (air-sea interface) Contribution of ships to PAHs in coastal regions Decision support for regulating authorities Main objectives

5. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante Benzo(a)Pyrene often chosen as a lead substance for PAHs PAHs imperil humans and ecosystems – highly bioaccumulative (food chain) – persistent in various environmental compartments – significant adverse effects already at low doses (Chlorofiles: A few microgram per liter seawater is enough to cause problems in the growth of plankton) carcinogenic impair immune system impair reproduction Why PAHs ? B(a)P Object of international reduction conventions

6. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante MM5 Emissions additionally in preparation CLM of DWD (German Weather Service) own emission module for B(a)P Model set up for annual simulations model components CMAQ version 4.5 with GKSS B(a)P module MM5 embedded in ERA-40 data for retrospective runs

7. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante MM5: MRF PBL scheme Reisner 2 microphysics Kain and Fritsch 2 cumulus scheme Noah LSM 4D grid nudging (ERA40) BC from ERA 40 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) Model set up for annual simulations physical schemes and parameterisations

8. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante Emphasis on mass transfer of B(a)P between the gaseous and the particulate phase B(a)P partitioning B(a)P degradation in gas phase to be added

9. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante 18x18 km 2 grid 54x54 km 2 grid 30 vertical layers up to 100 hPa MM5 and CMAQ for annual simulations model domain

10. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante Residential heating Road transport Electricity generation Iron and steel production Incineration of household waste Ship engines Oil platforms Wildfires Emissions major sources PAHs are formed by any incomplete combustion B(a)P emissions in 2000

11. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante B(a)P emissions for 4 months around Kosetice, CZ, 2000 nitrogen, sulfur, VOCs and aerosols from IER Stuttgart (base EMEP and EPER) B(a)P emissions are based on annual gridded values from Denier van der Gon et al. (2005) Modifications for B(a)P: - annual cycle - weekly cycle - diurnal cycle residential heating: ac following temperature, wc, dc following CO industry: wc following NO road traffic: wc, dc following NO Emissions modelling approach

12. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante CMAQ results: B(a)P concentrations 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 for lowest layer

13. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante CMAQ results: B(a)P wet deposition total annual amount of emitted B(a)P was the same for both model runs (based on 2000 data)

14. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante CMAQ results vs. EMEP measurements: B(a)P concentrations stations, 2000 South East Germany 2-day means South West Sweden monthly means model measurements B(a)P [ngm -3 ] 0 0 2 4

15. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante Stationmeanrmsbiascorr IOA Northern Germany 0.100 0.639 0.555 0.681 0.473 Czech Republic 0.169 0.644 0.497 0.553 0.568 Finland 0.006 0.078 0.058 0.869 0.471 Lithuania 0.808 0.526 -0.453 0.715 0.495 South East Germany 0.722 0.730 0.097 0.739 0.784 South West Sweden 0.078 0.218 0.206 0.710 0.504 East Sweden 0.048 0.592 0.544 0.304 0.405 B(a)P in ng/m 3, CMAQ model results vs. EMEP measurements, statistical quality indicators times series year 2000 CMAQ results vs. EMEP measurements: B(a)P concentrations statistics

16. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante Illmitz, Austria, 117 m asl Mean (meas)8.55  g/m 3 bias1.15  g/m 3 rms error5.73  g/m 3 Correlation0.56 IOA0.73 Neuglobsow, Germany 62 m asl Mean (meas)6.99  g/m 3 bias8.68  g/m 3 rms error12.38  g/m 3 Correlation0.81 IOA0.63 CMAQ results vs. EMEP measurements: NO 2 concentrations stations, daily means 2000 model measurements model measurements NO 2 [  gm -3 ] 60 0 0

17. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante U-wind monthly mean of correlation and bias vs. radiosonde data sorted by station Check of meteorological model parameters vertical profiles 88 radiosonde stations from the igra data base V-wind

18. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante vessel movement database from Lloyds Marine Intelligent Unit (LMIU) for the year 2000. ship emission rates after Cooper and Gustafsson (2004) Ship emissions are expected to contribute to a large extent to the total emissions of polycyclic aromatic hydrocarbons (PAHs), especially in marine and coastal areas. PAHs from ship traffic ongoing PhD research project Goal: assessment of the contribution of ship emmissions to PAH concentrations and deposition Assessment of past and future relevance

19. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante Implementation of degradation in gas phase Interface between CLM and CMAQ under construction Assessment of the influence of ship emissions Long-term model runs covering several decades (1970 to 2005) Setting up different emission scenarios Simulations with climate scenarios (ECHAM 5/CLM to 2050) Further PAHs, nutrients, chemical aerosol composition Conclusions & Outlook B(a)P module has been added to CMAQ Annual runs have been conducted for Europe Comparison with measurements B(a)P in general too high conc. but satisfactory correlations NO 2 in general good agreement PM10 lower than measurements ? B(a)P Emissions ?

20. Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante Thank You ! Questions ?