Emissions data for of heavy metal and POP modelling

TFEIP Workshop, Istanbul, May 2013

Emissions data for of heavy metal and POP modelling

Oleg Travnikov, Alexey Gusev, Ilia Ilyin, Olga Rozovskaya, Victor

Shatalov


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


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


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


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


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


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


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


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)


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)


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)


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)


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


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


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)


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


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


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


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)


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

Emissions data for of heavy metal and POP modelling

Documents

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