emissions data for of heavy metal and pop modelling
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TFEIP Workshop, Istanbul, May 2013
Emissions data for of heavy metal and POP modelling
Oleg Travnikov, Alexey Gusev, Ilia Ilyin, Olga Rozovskaya, Victor
Shatalov
TFEIP Workshop, Istanbul, May 2013
Requirements to emissions data for modelling
• Spatially resolved data for the whole EMEP region
• Multi-year emissions for assessment of long-term trends
• Additional emission parameters:- Chemical speciation and congener composition- Temporal variation of emissions- Height of emission sources
• Historical emissions and emissions to other media for multi-media modelling
• Emissions in other regions/continents for assessment of intercontinental transport
TFEIP Workshop, Istanbul, May 2013
EMEP officially reported emissions data
0
20
40
60
80
100
Aus
tria
Bel
arus
Bul
garia
Cro
atia
Cyp
rus
Cze
ch R
epub
licD
enm
ark
Est
onia
Fin
land
Fra
nce
Ger
man
yH
unga
ryIr
elan
dLa
tvia
Liec
hten
stei
nM
aced
onia
Mon
aco
Net
herla
nds
Nor
way
Pol
and
Por
tuga
lR
ep. o
f Mol
dova
Ser
bia
Slo
veni
aS
pain
Sw
eden
Sw
itzer
land
Uni
ted
Kin
gdom Ita
lyM
onte
negr
oA
lban
iaS
lova
kia
Rus
sian
Fed
erat
ion
Mal
taLi
thua
nia
Rom
ania
Ukr
aine
Luxe
mbo
urg
Bel
gium
Arm
enia
Kyr
gyzs
tan
Gre
ece
Aze
rbai
jan
Bos
nia
& H
erz.
Geo
rgia
Icel
and
Kaz
akhs
tan
Taj
ikis
tan
Tur
key
Tur
kmen
ista
nU
zbek
ista
n
Da
ta c
om
ple
ten
ess
, %
Completeness of reported HMs emission totals for 1990-2011
Complete datasets of emission totals are available for 28 countries
There is no national emissions data for 9 EMEP countries
TFEIP Workshop, Istanbul, May 2013
EMEP officially reported emissions data
0
20
40
60
80
100
Aus
tria
Bul
garia
Cro
atia
Cyp
rus
Den
mar
kE
ston
iaF
inla
ndF
ranc
eG
erm
any
Hun
gary
Icel
and
Irel
and
Latv
iaN
ethe
rland
sP
olan
dP
ortu
gal
Rep
. of M
oldo
vaS
erbi
aS
love
nia
Spa
inS
wed
enU
nite
d K
ingd
om Italy
Mon
tene
gro
Alb
ania
Bel
arus
Slo
vaki
aLi
echt
enst
ein
Mon
aco
Nor
way
Sw
itzer
land
Cze
ch R
epub
licB
elgi
umR
oman
iaR
ussi
an F
eder
atio
nLi
thua
nia
Luxe
mbo
urg
Geo
rgia
Mal
taU
krai
neM
aced
onia
Arm
enia
Kyr
gyzs
tan
Aze
rbai
jan
Bos
nia
& H
erz.
Gre
ece
Kaz
akhs
tan
Tur
key
Taj
ikis
tan
Tur
kmen
ista
nU
zbek
ista
n
Da
ta c
om
ple
ten
ess
, %
Completeness of reported POPs emission totals for 1990-2011
Complete datasets of emission totals are available for 22 countries
There is no national emissions data for 8 EMEP countries
TFEIP Workshop, Istanbul, May 2013
Data completeness: Emission sectors
Contribution of major source categories to HCB emissions
Public electricity and heat production (1A1a)
Road transport (1A3)
Iron and steel production (2C1)
Agriculture (4G)
Waste incineration (6C)
Other
France Spain United Kingdom
TFEIP Workshop, Istanbul, May 2013
EMEP domain
Spatial distribution and gaps filling
- National totals - TNO totals
t cell-1 y-1
Emission totals:
Reported data (40 countries)
TNO inventory for 2000 and projections for 2010
Gridded data:
Reported grids (27 countries)
TNO inventory for 2000 and projections for 2010
CGEIC global Pb emissions inventory (1°×1°) for 1989 scaled to present
Example: Pb anthropogenic emissions in 2011
TFEIP Workshop, Istanbul, May 2013
0%
20%
40%
60%
80%
100%
HgHCB
PCDD/Fs
BaPPCB Pb Cd
Contribution of regional vs. global sources to HM and POP pollution
Global sources
EMEP sources
Hg deposition over the globe and in EMEP region (2010)
Global sources and intercontinental transport
TFEIP Workshop, Istanbul, May 2013
Available ‘expert estimates’Dataset Chemicals Years Resolution
Europe
TNO inventory Pb, Cd, Hg, BaP, PCDD/Fs,
HCB
2000, 2010/20
(projections)
50×50 km2
POPCYCLING-Baltic
BaP, PCDD/Fs, HCB
1970-1995 50×50 km2
ESPREME Pb, Cd, Hg, … 2000 50×50 km2
DROPS PCDD/Fs, PCBs 2000 50×50 km2
Global
NILU/CGEIC Pb 1989 1°×1°
AMAP/UNEP Hg 2010 0.5°×0.5°
Tao et al., 2009 PAHs 2004 n/a
Bailey et al., 2001
HCB 1995 n/a
NILU inventory PCBs 1930-2100 1°×1°
No global data for Cd and PCDD/Fs
TFEIP Workshop, Istanbul, May 2013
Chemical speciation of emissions: Hg
Hg species: Hg0, Hg(II)gas, Hg(II)part
Reported emissions: total Hg
Expert estimates: Axenfeld et al., 1991; Pacyna et al., 2001
Effect of emission speciation on Hg deposition (2010)
All Hg emissions as Hg0 All emissions as Hg(II)
TFEIP Workshop, Istanbul, May 2013
Chemical speciation of emissions: PAHs
PAH indicator compounds: B[a]P, B[b]F, B[k]F, IP
Reported emissions: depends on a country
Expert estimates: TNO inventory
No data5 countries (11%)
All 4 PAHs30 countries (64%)
Only some PAHs5 countries (11%)
Sum of 4 PAHs7 countries (14%)
Reporting of PAHs emissions (2011)
TFEIP Workshop, Istanbul, May 2013
Chemical speciation of emissions: PCDD/Fs
PCDD/F composition: 17 toxic congeners
Reported emissions: total toxicity equivalent
Expert estimates: POPCYCLING-Baltic project
0%
5%
10%
15%
20%
TC
DF
12
Pe
CD
F2
3P
eC
DF
14
HxC
DF
16
HxC
DF
23
HxC
DF
19
HxC
DF
78
Hp
CD
F8
9H
pC
DF
OC
DF
TC
DD
Pe
CD
D4
HxC
DD
6H
xCD
D
7H
xCD
DH
pC
DD
OC
DD
40%
Congener composition of PCDD/Fs emissions (EMEP region)
TFEIP Workshop, Istanbul, May 2013
Temporal variation of emissions
Sectors of BaP emissions in EMEP countries (2010)
0%
20%
40%
60%
80%
100%
Others
Waste incinerationIndustrial processesRoad transportResidential heating
Industry and road transport (Schaap et al., 2005)
0
5
10
15
20
Jan
Fe
b
Ma
r
Ap
r
Ma
y
Jun
Jul
Au
g
Se
p
Oct
No
v
De
c
Em
issi
on
s, t
/mo
nth
Industrial processes
Road transport
0.0
0.1
0.2
0.3
0.4
Em
issi
on
s, m
g/m
2/d
ay
Jan
De
c
No
v
Oct
Se
p
Au
g
Jul
Jun
Ma
y
Ap
r
Ma
r
Fe
b
Residential heating (Aulinger et al., 2010)
Single location in Czech Republic
Seasonal variation of BaP air concentration at Kosetice (CZ3)
0.0
0.2
0.4
0.6
0.8
1.0
Jan
Fe
b
Ma
r
Ap
r
Ma
y
Jun
Jul
Au
g
Se
p
Oct
No
v
De
c
Ba
P a
ir c
on
cen
tra
tion
, ng
/m3 Observations
No variation
Observations
Model (no variation)
0.0
0.2
0.4
0.6
0.8
1.0
Jan
Fe
b
Ma
r
Ap
r
Ma
y
Jun
Jul
Au
g
Se
p
Oct
No
v
De
c
Ba
P a
ir c
on
cen
tra
tion
, ng
/m3 Observations
No variation
Observations
Model (emission)
TFEIP Workshop, Istanbul, May 2013
Arcelor-Mittal Ostrava Steel PlantEmission: 859 kg/y (26%)
Prunéřov II Power StationEmission: 207 t/y (6%)
Contribution (%)
Contribution of large point sources to Cd deposition
Note: Contribution of single LPS can exceed 10-20% of Cd total anthropogenic deposition over large areas of the country
Emissions from large point sources
TFEIP Workshop, Istanbul, May 2013
h
Required parameters: Stack height Stack diameter Gas outflow velocity Gas temperature
Emissions from large point sources
0
300
600
900
1200
1500
Jan
Fe
b
Ma
r
Ap
r
Ma
y
Jun
Jul
Au
g
Se
p
Oct
No
v
De
c
Em
issi
on
he
igh
t, m
Prunéřov II Power Plant
Estimates of effective emissions height (Brigg’s
approach)
Stack height - 300 m
Change in annual Pb deposition due to vertical redistribution of
emissions Percents
TFEIP Workshop, Istanbul, May 2013
HCB air concentration (2011)
EMEP anthropogenic
sources
Global anthropogenic
sourcesGlobal
secondary sources
EMEP secondary
sources
EMEP
Historical emissions of POPs
0%
20%
40%
60%
80%
100%
19
45
19
50
19
55
19
60
19
65
19
70
19
75
19
80
19
85
19
90
19
95
20
00
20
05
20
10
AirSoilOcean
HCB accumulation in different media
0
5
10
15
20
19
45
19
50
19
55
19
60
19
65
19
70
19
75
19
80
19
85
19
90
19
95
20
00
20
05
20
10
HC
B e
mis
sio
n, k
t/y
0.0
0.1
0.2
0.3
19
90
19
95
20
00
20
05
20
10
HCB global emissions (1945-2010)
TFEIP Workshop, Istanbul, May 2013
Emissions of POPs to other media
PCDD/Fs emissions in Europe(17 EU countries)
to land85%
to air15%
[Wenborn et al., 1999]
PCDD/Fs emissions to land
0 5 10 15
Emission to land, kg I-TEQ
Pesticide production
Accidental fires
Waste incineration
Waste disposal
Pesticide use
Other
PCDD/F air concentration(model vs. observations)
0.1
1
10
100
1000
0.1 1 10 100 1000
Observed, fg TEQ/m3M
od
elle
d,
fg T
EQ
/m3
Emission to air only
0.1
1
10
100
1000
0.1 1 10 100 1000
Observed, fg TEQ/m3M
od
elle
d,
fg T
EQ
/m3
Emission to air only
Emission to air & soil
Underestimation by a factor of
5
TFEIP Workshop, Istanbul, May 2013
Pb concentration in air (2007)
0
3
6
9
12
15
Jan
Fe
b
Ma
r
Ap
r
Ma
y
Jun
Jul
Au
g
Se
p
Oct
No
v
De
c
Pb
conc
entr
atio
n, n
g/m
3Observed
Model
0
3
6
9
12
15
Jan
Fe
b
Ma
r
Ap
r
Ma
y
Jun
Jul
Au
g
Se
p
Oct
No
v
De
c
Pb
conc
entr
atio
n, n
g/m
3Observed
Model
Optimized
Adjoint modelling Application of adjoint modelling for evaluation of emission
fields
Košetice (CZ3)
Adjoint model:
An adjoint model to a CTM provides estimates of spatially resolved influence functions ∂C/∂E for a chosen receptor:
Applied approach:
• Model simulation of influence functions for particular receptor
• Analysis of the optimized fields from the view point of possible emission uncertainties
• Variational optimization of emission fields to minimize model-measurement discrepancies at selected receptor
ij
ijijR ΔEECΔC
Influence function for CZ3
October 2007
Influence function
CZ3
TFEIP Workshop, Istanbul, May 2013
What can be improved?
Officially reported data:
• Completeness of national totals and gridded emissions
• Emissions differentiation by source categories and coverage of all emission sectors
• Information on large point sources (emissions, co-ordinates, height, etc.)
• Projections of future emissions
• Uncertainty estimates or lower/upper limits
TFEIP Workshop, Istanbul, May 2013
What can be improved?
Expert estimates:
• Updated inventories for EMEP countries and non-EMEP regions
• Global scale emissions data (Hg, HCB)
• Chemical speciation or congener composition of emissions (Hg, PCDD/Fs, PAH, PCBs)
• Temporal variation of emissions (e.g. by sectors)
• Historical emissions (HCB, PCDD/Fs, Hg)
• Emissions to other media (soil, water)
TFEIP Workshop, Istanbul, May 2013
0
3
6
9
12
15
Jan
Fe
b
Ma
r
Ap
r
Ma
y
Jun
Jul
Au
g
Se
p
Oct
No
v
De
c
Pb
conc
entr
atio
n, n
g/m
3
Observed
Model
Pb concentration in air (2007)
0
3
6
9
12
15
Jan
Fe
b
Ma
r
Ap
r
Ma
y
Jun
Jul
Au
g
Se
p
Oct
No
v
De
c
Pb
conc
entr
atio
n, n
g/m
3
Observed
Model
Optimized
Optimized (anthrop.)
Application of adjoint modelling Optimization of HM anthropogenic emissions distribution
Changes of total Pb emission
0
200
400
600
Polan
dIta
ly
Franc
e
Ger
man
y
Slova
kia
Belgiu
m
Czech
Rep
.
Nethe
rland
s
Hunga
ry
Switzer
land
Austri
a
Pb
emis
sion
s, t/
y Original
Optimized
October 2007
Influence function
CZ3
Optimization coefficients
CZ3
Anthrop. emissions
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