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 ResearchGKSS Research CenterGeesthacht, Germany

Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante

GKSS is member of the Helmholtz Association

Material ResearchPolymer ResearchCoastal Research

GKSS Research Center

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

Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante

Estimation and assessment of depositions andconcentration levels of PAHs in coastal ecosystemsat 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 regionsDecision support for regulating authorities

Main objectives

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

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 simulationsmodel components

CMAQ version 4.5 with GKSS B(a)P module

MM5 embedded in ERA-40 data for retrospective runs

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 simulationsphysical schemes and parameterisations

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

Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante

18x18 km2 grid

54x54 km2 grid 30 vertical layers up to 100 hPa

MM5 and CMAQ for annual simulationsmodel domain

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

Emissionsmajor sources

PAHs are formed by any incomplete combustion

B(a)P emissions in 2000

Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante

0 10 20 300

0.01

0.02

0.03

0.04

B(a

)P e

mis

sion

[g

s-1]

100 110 120 190 200 210 280 290 300

Julian D ay

January April Ju ly O ctober

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

Emissionsmodelling approach

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

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)

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

model

measurements

measurements

B(a)P [ngm-3]

B(a)P [ngm-3]

0

0

2

4

Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante

Station mean rms bias corr IOA Northern Germany 0.100 0.639 0.555 0.681 0.473Czech Republic 0.169 0.644 0.497 0.553 0.568Finland 0.006 0.078 0.058 0.869 0.471Lithuania 0.808 0.526 -0.453 0.715 0.495South East Germany 0.722 0.730 0.097 0.739 0.784South West Sweden 0.078 0.218 0.206 0.710 0.504East Sweden 0.048 0.592 0.544 0.304 0.405

B(a)P in ng/m3, CMAQ model results vs. EMEP measurements, statistical quality indicators

times series year 2000

CMAQ results vs. EMEP measurements: B(a)P concentrations

statistics

Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante

Illmitz, Austria, 117 m aslMean (meas) 8.55 g/m3

bias 1.15 g/m3

rms error 5.73 g/m3

Correlation 0.56IOA 0.73

Neuglobsow, Germany 62 m aslMean (meas) 6.99 g/m3

bias 8.68 g/m3

rms error 12.38 g/m3

Correlation 0.81IOA 0.63

CMAQ results vs. EMEP measurements: NO2 concentrations

stations, daily means 2000model

measurements

model

measurements

NO2 [gm-3]

NO2 [gm-3]

60

60

0

0

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 parametersvertical profiles

88 radiosonde stations from the igra data base

V-wind

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 trafficongoing PhD research project

Goal:

assessment of the contribution of ship emmissions to PAH concentrations and deposition

Assessment of past and future relevance

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

NO2 in general good agreement

PM10 lower than measurements ? B(a)P Emissions ?

Models-3 Workshop, Swindon, UK, 13.03.2007 Markus Quante

Thank You !

Questions ?