focus on the Mediterranean and the

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Atmospheric deposition of nitrogen
and sulfur over Southern Europe with
focus on the Mediterranean and the
Black
Sea:
WRF/CMAQ modeling

U. Im
1,2
, S. Christodoulaki
1,3
, K. Violaki
1
, P. Zarmpas
1
, M.
Kocak
4
, N. Daskalakis
1,2
,
N. Mihalopoulos
1
, M.
Kanakidou
1


[1] Environmental Chemical Processes Laboratory, Department of Chemistry, University of
Crete, Voutes Campus, P.O.Box 2208, 71003, Heraklion, Greece

[2] Institute of Chemical Engineering Sciences, Foundation for Research and Technology
Hellas (FORTH), Patras, Greece

[3] Institute of Oceanography, Hellenic Center for Marine Research, P.O. Box 2214, 71003,
Heraklion, Crete, Greece

[4] Institute of Marine Sciences, Middle East Technical University, Erdemli, Mersin,
Turkey

Paper , under review
Atmos

Environ, 2013

INTRODUCTION


Nitrogen (N) and Sulfur (S) impact on:


Atmospheric chemistry (O
3

chemistry, SIA


HNO
3
, H
2
SO
4
)


Ecosystem (deposition: fertilization, acidification and accumulation)


N and S have both anthropogenic and natural sources


Emissions and deposition of N/S species will further
increase/decrease in the future.







2

BACKGROUND

Duce et al., Science, 2008

ACCENT 2013, September 2013, Urbino, Italy

Chl

“a” distribution along Mediterranean

Europe’s Environment, 1998.

N/P ratio in seawater from 22
-
28 >> than the normal (18)

MOTIVATION

HNO
3

NH
3

NO
3
-

NH
4
+

Dry
Deposition

Wet
Deposition

NO
3
-

NH
4
+

Total
Depositio
n

NO
3
-

NH
4
+

NO
x

NO
y

Particulate Nitrogen

500 m

1500 m

Sediment traps

Mesozooplancton

Phytoplanton

Bacteries

Cilies

MOTIVATION

0
1
2
3
4
1
2
3
4
5
6
7
8
9
10
11
12
Months
mmolN/
(15d*m
2
)
Sediment traps
Dry deposition
Wet deposition
Kouvarakis

et al., GBC, 2001

MOTIVATION


The

results

obtained

during

this

study

showed

that

airborne

DIN

alone

is

more

than

sufficient

to

explain

new

production

in

the

East

Mediterranean

Sea
.

Dry

deposition

alone

accounts

for

about

a

factor

of

two

of

the

collected

PON

and

both

dry

and

wet

deposition

account

for

about

370
%

of

the

PON
.



Observations

have

limited

geographical

coverage
.



CTMs

provide

integrated

view

(temporal

and

spatial

variations)

(local

to

global)
.



Few

modeling

studies

dedicated

to

the

atmospheric

deposition

of

N

and

S

to

the

Mediterranean

and

the

Black

Seas
.

FOCUS ON MEDITERRANEAN & BLACK SEA

METHODS


MODEL CONFIGURATION


WRF/CMAQ


171
×
123
×
23 grid cells


30 km horizontal resolution


Vertical extent ~16 km


CB
-
V chemical mechanism
(
Yardwood et al., 2005
)


AERO5 aerosol mechanism (
Foley et
al.,
GeosciModDev
, 2010
)


NCEP meteorology for 2008


Monthly mean chemical boundary
conditions (global model TM4
-
ECPL:
Myriokefalitakis et al., ACP, 2011)


Model setup:
Im and Kanakidou,
ACP, 2012 & Im et al STOTENV,
under review, 2013


Natural Emissions and Biomass
burning Emissions are calculated on
line.

7

WRF
METEOROLOGICAL
MODEL

INITIAL/BOUNDARY
CONDITIONS (TM4
-
ECPL)

MOSSES
ANTHROPOGENIC
EMISSIONS MODEL

CHEMISTRY AND
TRANSPORT MODEL
(CMAQ)

NATURAL EMISSIONS
(MEGAN
BIOGENIC+GOCART
DUST)


NCAR FINN BIOMASS
BURNING EMISSIONS
MODEL

ACCENT 2013, September 2013, Urbino, Italy

EMISSIONS

Sectors

(tons/yr)

NO
x

NH
3

SO
2

Anthropogenic

1.7E+7

5.7E+6

1.4E+7

Biogenic

6.8
E+
5

Biomass Burning

2
.2
E+3

8.7
E+2

1.9E+2

8

Anthropogenic Emissions



INERIS 10 km inventory for Europe


CIRCE global emissions for remaining



parts around the Mediterranean and



Asia (
Pozzer

et al., ACP, 2012
)


2 km emissions for Istanbul (
Markakis



et al., APR 2012
) and Athens
(
Markakis et al., WASP & APR, 2010
)

Im et al. (2013)
AtmEnv
. Under Review

ANNUAL TOTAL N & S EMISSIONS

ANNUAL SECTORAL N EMISSIONS

ACCENT 2013, September 2013, Urbino, Italy

OBSERVATIONS

9

Im et al. (2013)
AtmEnv
. Under Review

EMEP
wet deposition: 45
stations, 2008

http://www.emep.int/


Mihalopoulos

unpublished
data
: 2008. Finokalia station,
Greece, dry deposition
http://finokalia.chemistry.uoc.gr


Medinets

and
Medinets
,
TurJFishAqua
, 2012
: Zmiinyi
station, Black Sea, 2008


Markaki
et
al.,
MarChem
,
2010
:5 stations 2001
-
2003


Kocak et al.,
BioGeoSci
,
2010
: Erdemli, Turkey
station, 2006
-
2007




ACCENT 2013, September 2013, Urbino, Italy

10

MODEL VALIDATION



r
2

Bias

NMB

RMSE

IOA

MAGE

NM
E

NH
4
+

0.3

-
198

-
53

262

0.6

201

54

NO
3
-

0.4

-
47

-
17

146

0.8

110

39

NH
4
+
+
NO
3
-

0.4

-
165

-
47

226

0.7

170

48

SO
4
=

0.2

-
125

-
36

267

0.6

172

46

Preci
p

0.5

-
116

-
12

417

0.8

318

33

10

COMPARISON* WITH EMEP
WET DEPOSITION, 2008

PRECIPITATION

SO
4
=

NO
3
-

NH
4
+

*Statistics are based on daily mean data

ACCENT 2013, September 2013, Urbino, Italy

ANNUAL DEPOSITION FLUXES

Normalized mean error between
modeled &observed N deposition fluxes
(N*: Total N as in the observations)

100
1
1







N
i
i
N
i
i
i
O
O
P
NME
N DEPOSITION OVER EUROPE, THE
MEDITERRANEAN & THE BLACK SEA



Nitrogen
deposition
(Tg
-
N

yr
-
1
)

Precip.

(mm

yr
-
1
)

Nitrogen

Emis
.(Tg
-
N

yr
-
1
)

Deposition


Emission



Dry

Wet

Total

Sea

Land
+Sea

Sea

Land
+Sea

Sea

Land+
Sea

Sea

Land+Sea

BS

0.23

0.12

0.36

415

0.52

0.7

EM

0.81

2.88

0.29

0.85

1.10

3.73

349

405

2.88

1.3

WM

0.60

2.80

0.32

0.65

0.92

3.45

491


384

1.93

1.8

E
urope

4.14

5.65

0.75

2.03

4.89

7.68

504


555

9.26

0.8

11

ACCENT 2013, September 2013, Urbino, Italy

S
DEPOSITION OVER EUROPE, THE
MEDITERRANEAN & THE BLACK SEA

ACCENT 2013, September 2013, Urbino, Italy

12



Sulfur

deposition
(
Tg
-
S

yr
-
1
)

Precip.

(mm

yr
-
1
)

Sulfur

Emis
.(
Tg
-
S

yr
-
1
)

Deposition


Emission



Dry

Wet

Total

Sea

Land
+Sea

Sea

Land+
Sea

Sea

Land+
Sea

Sea

Land+
Sea

BS

0.
16

0.01

0.
17

415

0.
40

0.4

EM

0.
52

1.37

0.
32


0.
70

0.84


2.07

349

405

2.88

0.7

WM

0.
33


0.48

0.
19


0.
33

0.
52


0.81

491


384

0.84

1.0

E
urope

1.59


2.51

0.
49


1.37

2.07

3.88

504


555

5.08

0.8

IMPORTANCE & IMPACTS OF N DEPOSITION

LAND


19
% of total N
(0.93
Tg
-
N
yr
-
1
) is deposited



over forests.


84
% of the forested
regions receive


fluxes larger
than the critical



nitrogen
load of
1
g
-
N m
-
2

yr
-
1
.




OCEAN


13

N (g
-
N m
-
2

yr
-
1
)

Annual N deposition over forests

Atm
=2.02
TgN

yr
-
1

ASW=1.4
TgN

yr
-
1

River=1.08
TgN

yr
-
1

GW=0.3
TgN

yr
-
1

ACCENT 2013, September 2013, Urbino, Italy

IMPACTS OF N DEPOSITION OVER
MARINE ECOSYSTEMS

14



The excess of N accumulates then in the water column and could explain the
anomalous N/P ratio observed in the Eastern Mediterranean (
Christodoulaki

et al.,
JMarineSys
, 2013
).

Atm. N Dep.

0.36 TgN yr
-
1

N

C


C production


2.4 TgC yr
-
1


Sedimentation


1.6 TgC yr
-
1

Theodosi et al.,
BioGeoSciDisc
, 2013


BLACK SEA

Atm. N Dep.

0.8 g N m
-
2

yr
-
1

N


Sedimentation


0.16 gN m
-
2

yr
-
1

Kouvarakis et al., GBC,
2001


EAST MED. SEA

ACCENT 2013, September 2013, Urbino, Italy

CONCLUSIONS


The Mediterranean Sea receives 2.02 Tg
-
N yr
-
1

and
1.36
Tg
-
S
yr
-
1
while the Black Sea receives 0.36
Tg
-
N yr
-
1
and

0.17
Tg
-
S
yr
-
1
.


Results compare reasonably with observations and previous model
studies over Europe although some underestimation is seen
depending
on species and
season.


A
significant amount of the
deposited N and S is
transported
to
the
Mediterranean
basin.


The
critical
nitrogen load (1
g
-
N m
-
2

yr
-
1
)

is
exceeded
in 84%
of the
European forested
areas.



Atmospheric deposition plays a predominant role
on
the open
Mediterranean and Black
Seas ecosystems functioning.


Excess N accumulates in the East Med Sea
due to atmospheric N
and is leading to high N/P ratios.


15

ACCENT 2013, September 2013, Urbino, Italy

THANK YOU

ACCENT 2013, September 2013, Urbino, Italy

16

ACKNOWLEDGEMENTS

U. Im

N. Daskalakis

M. Kanakidou

S.
Christodoulaki

N. Mihalopoulos

K.
Violaki

PEGASOS

FOCUS ON MEDITERRANEAN & BLACK SEA


Pollution receptor regions, seasonality.


Semi
-
closed ecosystem


East Mediterranean Sea is oligotrophic








Observations have limited geographical coverage.


CTMs provide integrated view (temporal and spatial variations) (local
to global).


Few modeling studies dedicated to the atmospheric deposition of N
and S to the Mediterranean and the Black Seas.


18

Lelieveld et al., Science, 2002

MOTIVATION

ACCENT 2013, September 2013, Urbino, Italy