modelling of mercury, lead and cadmium at european scale

Modelling of mercury, lead andcadmium at european scale.

Yelva Roustan

[email protected]

Modelling of mercury, lead and cadmium at european scale. – p. 1/17

Introduction

I Long lived species, harmfull and bioaccumulable

I Convention on Long-Range Transboundary AirPollution (Geneva, 1979)

. Protocol on Heavy Metals (Aarhus, 1998)

• continental scale

• long-term simulation


Models


Models: lead and cadmium

concentration

Pb 1-10 ng.m−3

Cd 0.1-1 ng.m−3

life time

days to weeks

. size distribution

. deposition process0.001 0.01 0.1 1 10 100

µm

1e-08

1e-06

1e-04

0.01

1

1/s

P0 = 1 mm/hP0 = 10 mm/hP0 = 50 mm/h

0.001 0.01 0.1 1 10 100µm

0.01

0.1

1

10

100

cm/s

vent = 1 m/svent = 2 m/svent = 5 m/svent = 10 m/s


Models: mercuryconcentration life time

Hg0 1.5-2 ng.m−3 months

HgII 10-100 pg.m−3 hours to days

Hgp 10-100 pg.m−3 days to week

. chemical process

Petersen 1995 Ryaboshapko 2002


Simulations


Simulations: lead and cadmiumair concentration site wet deposition site

1 10Observation

1

10

Mo

del

-+ 75%-+ 50% 1 diameter10 diameters

Pb in air

0.1 1 10Observation

0.1

1

10

Pb wet flux

0.1 1Observation

0.1

1

Cd in air

1 10 100Observation

1

10

100

Mo

del

Cd wet flux


Simulations: cadmiumAir concentration (ng.m−3)

! " ! # ! !

$%$&

'(' $

')'%

'&) (

) $

*+, -. +, -

/ +, -0 +, -

1 +, 2 +, 1 +, 3 4 +, 3 5 +, 3 * +, 3

67 867 9

67 :67 ;

67 <67 =

67 >67 ?

67 @

1 diameter - (a)fractional bias

(a) - (b)10 diameters - (b)

ABC DE BC D

F BC DG BC D

H BC I B C H B C J K BC J L B C J AB C J

MNON

PNQN

RNSN

TNM MN

M QN

UVW XY VW X

Z VW X[ VW X

\ VW ] V W \ VW ^ _ VW ^ `V W ^ UVW ^

a bca dc

a eca f c

a g ca b

cb

g c

hij kl ij k

m ij kn ij k

o ij p ij o ij q r ij q s ij q h ij q

tuvu

wuxu

yuzu

ut tu

t xu

Total deposition flux (g.km−2.y−1)


Total gaseous mercury concentration (ng.m−3)

annual mean monthly mean

J F M A M J J A S O N D1

1.5

2

2.5

ObservationPolair3D - v1Polair3D - v2

IE31 - Mace Head


1.5

2

2.5

FI96 - Pallas


1.5

2

2.5

NO99 - Lista


1.5

2

2.5

SE02 - Rorvik

POLAIR3D - v1 POLAIR3D - v2

IE31 FI96 NO99 SE02 IE31 FI96 NO99 SE02

observation 1,65 1,33 1,63 1,67 1,65 1,33 1,63 1,67

model 1,85 1,63 1,85 2,05 1,77 1,59 1,71 1,76

fractional bias -12 -20 -13 -21 -7 -18 -5 -7


Mercury deposition flux (g.km−2.y−1)

total deposition - annual mean wet deposition - monthly mean

ObservationPolair3D "corrected"Polair3D

SE11SE05048

12162024

SE02

0

0.1

0.2

0.3

0

4

8

12

16

20

24

DE01

0

0.1

0.2

0.3

J F MA M J J A S OND

ObservationECMWF data

DE09

J FMAM J J A SOND

NL91

J FMAM J J A SOND

04812162024

NO99

0

0.1

0.2

0.3

J F MA M J J A S OND

Deposition flux( g/km²/year)

Precipitation( mm/h )

DE01 DE09 NL91 NO99 SE02 SE05 SE11

observation 4,4 6,2 9,1 8,9 5,4 3,6 4,7

POLAIR3D - v2 8,1 7,7 9,7 5,4 6,0 3,1 7,7

fractional bias -58 -22 -16 52 -7 20 -47


Sensitivity analysis


Sensitivity analysistransport equation: Ω = D × [0, τ ]

∂c

∂t+ div (uc) − div (K∇c) + Λ c + M c = σ

measurement equation:

µi =

∫

Ω

dtdx 〈πi(x, t), c(x, t)〉

adjoint equation:

−∂c

∗i

∂t−div (uc

∗i )−div (K∇c

∗i )+Λc

∗i +M

Tc∗i = πi


Sensitivity analysis

Contributions to the modelled measurement:

µi =

∫

Ω

dtdx 〈c∗i ,σ〉

︸︷︷︸

volume emission

+

∫

∂Ω0

dx 〈c∗i , c〉

︸︷︷︸

initial condition

+

∫

∂Ωb

dtdS · 〈c∗i ,E〉

︸︷︷︸

surface emission

−

∫

∂Ω+

dtdS · (〈c∗i , c〉u)

︸︷︷︸

boundary conditions


Sensitivity analysis: applications

sensitivity to boundary

and initial conditions

sensitivity to emissions

annual modelled measurement

monthly modelled measurement

log10( s / smax) s : average sensitivitysmax : maximum over the domain of s


Sensitivity analysis: applicationsTransboundary Pollution

example: Germany 2001January

February

! "#$

! "! % #$

! %! & #$

! &! ' #$

! '! ( #$

March

)*+ ,

- *+ ,

. *+ ,

/ *+ ,0 *+ 1 *+ 0 *+ 2 3 *+ 2 4 *+ 2

5 678

5 65 9 78

5 95 : 78

5 :5 ; 78

5 ;5 < 78

log10( s / smax) s : average sensitivitysmax : maximum over the domain of s


Model applicationImpact of EDF coal power plant

Mercury

Lead

Cadmium

! "# $% "# $

& "# $' "# $

( "# ) "# ( "#* + "#* , "#* ! "#*

-. - - -/

-. - -0-. - - /

-. -0-. -/

-. 0-. /

0/

Difference (in %) in the modeled deposition field due to theemission of the power plant (EMERAUDE).


ConclusionI Heavy metal models

Roustan, PhD Thesis, 2005

I Sensitivity analysisRoustan and Bocquet, Journal of Geophysical Research 2006

I Inverse modellingRoustan and Bocquet, Atmospheric Chemistry and Physics 2006

. Extension to a hemispherical domain

. Applications of the adjoint method

. Multi-media impact studySolen Queguiner, PhD Thesis

. Source-Receptor matrices


modelling of mercury, lead and cadmium at european scale

Documents