Modelling of BaP concentrations over France. Florian Couvidat Florian.Couvidat@ineris.fr

Simulations of BaP with Chimere Chimere was used to simulate BaP deposition over France watersheds Partitioning of BaP using its saturation vapor pressure (9.34 x 10-7 Pa) and degradation with OH (kinetic parameter of 5.00 x 10- 11 molecules-1 cm3 s-1) Annual emmissions from the French Emission Inventory (INS): 1 km Two studies with Chimere for year 2010: Europe 0.5° and France 0.07° Europe 0.25° and France 0.04° with the runoff coefficient to estimate the contribution of wet deposition to surface water concentrations

Low concentrations of BaP compared to other countries Results Similar results between EMEP and Chimere EMEP ng m-3 Chimere ng m-3 Low concentrations of BaP compared to other countries ng m-3

Contribution to groundwater Espèces Deposition kg/an Amount deposited in groundwater Industrial emissions in ground water BaP 4846 2364 ± 242 Between 2 and 45 kg/an BghiP 5484 2680 ± 274 Between 1 and 64 kg/an InD 3133 1529 ± 157 Between 0,4 and 39 kg/an Deposition kg/an Amount deposited in groundwater Industrial emissions in ground water BaP 4846 2364 ± 242 Between 2 and 45 kg/an BghiP 5484 2680 ± 274 Between 1 and 64 kg/an InD 3133 1529 ± 157 Between 0,4 and 39 kg/an

Measurements vs Model Correlation : 0.037

BaP~ f(emission, distance, altitude) Kriging : Obs + émissions + altitude Model Mean quadratic error by station type: Indust Rural Subur Traffic Urban 0.52 0.14 0.046 0.022 BaP~ f(emission, distance, altitude) Average: 0.17 Mean quadratic error divided by kriging variance: Indust Rural Subur Traffic Urban 7.0 1.9 0.62 0.30 Average: 2.3 Cross Validation result: Cor=0.708 Observations BaP 2010 Kriging result

BaP~ f(emission, distance, altitude)+ population Kriging : Obs + emissions/distance + population Model Mean quadratic error by station type: Indust Rural Subur Traffic Urban 0.45 0.17 0.043 0.015 0.13 BaP~ f(emission, distance, altitude)+ population Average: 0.15 Mean quadratic error divided by kriging variance: Indust Rural Subur Traffic Urban 5.9 2.2 0.56 0.20 1.6 Average: 2.0 Cross Validation result: Cor=0.735 Observations BaP 2010 Kriging result

2012 (Guereiro et al, 2016 ) ~Emiss*altitude+pop CHIMERE Emissions

Are emissions underestimated over France??? Weak emissions of BaP in France BaP emissions EMEP for 2000: 7,9 T for France 7,5 T for Belgium 31 T for Germany Emissions TNO 83 T for France 51 T for Germany France and Germany : Official data Spain, Italy, Belgium: CEIP estimates

BaP from residential wood burning Residential wood burning is the main contributor to BaP emissions 67% for France and 83% for Germany with also 21% of BaP emissions from forest fires for France (not estimated for Germany) French emissions factors was estimated in 2000 by INERIS More recent devices seem to emit more BaP BaP/(RWB PM2.5) ratio (in T/kT)

New simulations New simulations: - with a saturation vapor pressure of 6,3 x 10-6 Pa (instead of 9.34 x 10-7 Pa) based on Efstathiou et al., 2016 - taking into account heterogeneous degradation with ozone - with or without a factor 10 of increased emissions of BaP

Station in the southeast Station near Belgium Station in the southeast

Conclusions Low emissions of BaP compared to the other countries giving strong differences in concentrations (that does not seem supported by measurements) Lack of correlation between high resolution simulations and measurements Hypothesis: underestimation of BaP emissions that could be due to the wrong trend (decrease instead of increase) coupled with a overestimation of emissions in neighbouring countries