EMEP Intercomparison Study of Numerical Models for Long ...Long-Range Atmospheric Transport of...

EMEP Intercomparison Study of Numerical Models for Long-Range Atmospheric Transport of Mercury

Summary presentedby Mark Cohen,

NOAA Air Resources Laboratory,

Silver Spring, MD, USA

EMEP/TFMM Workshop on the Review of the MSC-E Modelson HMs and POPsOct 13-14, 2005Hotel Mir, Moscow Russia


BudgetsDry DepWet DepRGMHg(p)Hg0Chemistry

Conclu-sions

Stage IIIStage IIStage IIntro-duction

2

ParticipantsD. Syrakov …………………………….. Bulgaria….NIMHA. Dastoor, D. Davignon ……………… Canada...... MSC-CanJ. Christensen …………………………. Denmark…NERIG. Petersen, R. Ebinghaus …………...... Germany…GKSSJ. Pacyna ………………………………. Norway…..NILUJ. Munthe, I. Wängberg ……………….. Sweden….. IVLR. Bullock ………………………………USA………EPAM. Cohen, R. Artz, R. Draxler ………… USA………NOAAC. Seigneur, K. Lohman ………………..USA……... AER/EPRIA. Ryaboshapko, I. Ilyin, O.Travnikov…EMEP……MSC-E



Conclu-sions


3

Intercomparison Conducted in 3 Stages

I. Comparison of chemical schemes for a cloud environment

II. Air Concentrations in Short Term Episodes

III. Long-Term Deposition and Source-Receptor Budgets



Conclu-sions


4

Stage

Hybrid Single Particle Lagrangian Integrated Trajectory model, US NOAAHYSPLIT

MSC-E heavy metal hemispheric model, EMEP MSC-EMSCE-HM-Hem

Acid Deposition and Oxidants Model, GKSS Research Center, Germany ADOM

MSC-E heavy metal regional model, EMEP MSC-EMSCE-HM

Community Multi-Scale Air Quality model, US EPACMAQ

Eulerian Model for Air Pollution, Bulgarian Meteo-serviceEMAP

Chemistry of Atmos. Mercury model, Environmental Institute, SwedenCAM

Mercury Chemistry Model, Atmos. & Environmental Research, USA MCM

Danish Eulerian Hemispheric Model, National Environmental Institute DEHM

Global/Regional Atmospheric Heavy Metal model, Environment CanadaGRAHM

IIIIII

Model Name and InstitutionModel Acronym

Participating Models



Conclu-sions


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6

Hg(II), Reactive Gaseous Mercury [RGM]Elemental Mercury [Hg(0)]

Particulate Mercury [Hg(p)]

Atmospheric Mercury

Re-emission of previously

deposited mercury

PrimaryAnthropogenic

Emissions

Naturalemissions Wet and Dry Deposition

CLOUD DROPLET

cloud

Hg(II) reduced to Hg(0) by SO2 and sunlight

Hg(0) oxidized to dissolved Hg(II) species by O3, OH,

HOCl, OCl-

Adsorption/desorptionof Hg(II) to/from soot

Hg(p)

Vapor phase Hg(0) oxidized to RGM and Hg(p) by O3,

H202, Cl2, OH, HCl Hg(p) Dissolution?



Conclu-sions


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Variation of Hg concentrations (ng/L)

0

20

40

60

80

100

120

140

160

TCM AER CAM MSC-E CMAQ

Models

Con

cent

ratio

n, n

g/L



Conclu-sions


8

Effect of Different Assumptions Regarding Hg(p) SolubilityAER/EPRI 0%; MSCE-EMEP 50%; CMAQ-EPA 100%

0

50

100

150

0 12 24 36 48

Hours

Con

cent

ratio

n, n

g/L

AER EPRIMSCE EMEPCMAQ EPA



Conclu-sions


9

Stage I Publications:2001 Ryaboshapko, A., Ilyin, I., Bullock, R., Ebinghaus, R., Lohman,

K., Munthe, J., Petersen, G., Seigneur, C., Wangberg, I. Intercomparison Study of Numerical Models for Long Range Atmospheric Transport of Mercury. Stage I. Comparisons of Chemical Modules for Mercury Transformations in a Cloud/Fog Environment. Meteorological Synthesizing Centre – East, Moscow, Russia.

2002 Ryaboshapko, A., Bullock, R., Ebinghaus, R., Ilyin, I., Lohman, K., Munthe, J., Petersen, G., Seigneur, C., Wangberg, I. Comparison of Mercury Chemistry Models. Atmospheric Environment 36, 3881-3898.

10



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11

SO3=, HO2SO3

=SO3=SO3

=SO3=, HO2SO3

=SO3=, hv, HO2

Liquid-phase reduction agents

O3O3O3O3O3, OH!, HOCl,

OCl-O3O3, OH!, HOCl, OCl-Liquid-phase oxidation agents

O3 (f)O3O3O3, OH!O3, H2O2,Cl2, HClO3O3, H2O2, Cl2, OH·Gas-phase oxidation

agents

200none10102017TPM boundary condition (pg/m3)

00none105217RGM boundary condition (pg/m3)

1.6 - 1.71.5No1.51.51.51.7Hg(0) boundary condition (ng/m3)

50 x 5050 x 50150 x 1501o x 1o50 x 5036 x 36,

108 x 10855 x 5536 x 36Horizontal resolution (km, unless noted differently)

3.915305151015Model top height (km)

SDA,NCEP/NCAR

reanalysis

NCEP / NCAR reanalysis

Canadian Meteorolo-gical Centre

SDA,NCEP/NCAR

reanalysis

NCEP/NCAR (MM-5)HIRLAMECMWF TOGA

reanalysis (MM5)Source of meteorological data

regional/EMEPHemisphericglobalregional/

EMEPregional/EMEP

regional/ Central Europe

regional/Central and

Northern Europe

Scale/Domain

EulerianEulerianEulerianEulerianLagrangianEulerianEulerianModel type

MSCE-HgDEHMGRAHMEMAPHYSPLITADOMCMAQ-HgModel



Conclu-sions


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Anthropogenic Mercury Emissions Inventoryand Monitoring Sites for Phase II

(note: only showing largest emitting grid cells)

Mace Head, Ireland grassland shore Rorvik, Sweden

forested shore

Aspvreten, Sweden forested shore

Zingst, Germanysandy shore

Neuglobsow, Germany forested area



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Neuglobsow

Zingst

AspvretenRorvik

Mace Head



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Total Gaseous Mercury at Neuglobsow: June 26 – July 6, 1995

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul 00.0

1.0

2.0

3.0

4.0

Tota

l Gas

eous

Mer

cury

(ng/

m3)

MEASURED

NWNW

NW

N

N

S

SE

NW

Neuglobsow



Conclu-sions


15

Total Gaseous Mercury (ng/m3) at Neuglobsow: June 26 – July 6, 1995

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul01234 MEASURED

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul01234 MSCE

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul01234 CMAQ

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul01234 GRAHM

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul01234 EMAP

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul01234 DEHM

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul01234 ADOM

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul01234 HYSPLIT



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Total Gaseous Mercury (ng/m3) at Neuglobsow: June 26 – July 6, 1995

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul01234 MEASURED

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul01234 MSCE

Using default emissions inventory

The emissions inventory is a critical input to the models…

26-Jun 28-Jun 30-Jun 02-Jul 04-Jul 06-Jul01234 MSCE - UBA

Using alternative emissions inventory



Conclu-sions


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Total Particulate Mercury (pg/m3) at Neuglobsow, Nov 1-14, 1999

02-Nov 04-Nov 06-Nov 08-Nov 10-Nov 12-Nov 14-Nov0

50

100

150MEASURED


50

100

150CMAQ


50

100

150GRAHM


50

100

150EMAP


50

100

150DEHM


50

100

150ADOM


50

100

150HYSPLIT


50

100

150MSCE

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MSCE Neuglobsow RGM

0

10

20

30

40

50

60

9 9 9 9 9 9 9 9 9 9 9 9 9 9

pg/m

3

ObsCalc

CMAQ Neuglobsow RGM

010203040506070

pg/m

3

ObsCalc

ADOM Neuglobsow RGM

010203040506070

pg/m

3

ObsCalc

EMAP Neuglobsow RGM

0

5

10

15

20

25

pg/m

3

ObsCalc

GRAHM Neuglobsow RGM

0

35

70

105

140

pg/m

3

ObsCalc

HYSPLIT Neuglobsow RGM

0

10

20

30

40

50

60

pg/m

3

ObsCalc



Conclu-sions


DEHM Neuglobsow RGM

0

6

12

18

24

30

pg/m

3

ObsCalc

Reactive Gaseous Mercury at Neuglobsow, Nov 1-14, 1999



Conclu-sions


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Overall Phase II statistics for 2-week episode means

0

20

40

60

80

100

De viatio n fac t

Perc

enta

ge, %

2 3 5 10

TGMTPM RGM

Deviation Factor

RGM: 90% within a factor of 10

RGM: 50% within a factor of 2

TPM: 90% within a factor of 2.5

TGM: all within a factor of 1.35



Conclu-sions


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Stage II Publications:2003 Ryaboshapko, A., Artz, R., Bullock, R., Christensen, J., Cohen, M.,

Dastoor, A., Davignon, D., Draxler, R., Ebinghaus, R., Ilyin, I., Munthe, J., Petersen, G., Syrakov, D. Intercomparison Study of Numerical Models for Long Range Atmospheric Transport of Mercury. Stage II. Comparisons of Modeling Results with Observations Obtained During Short Term Measuring Campaigns.Meteorological Synthesizing Centre – East, Moscow, Russia.

2005 Ryaboshapko, A., Bullock, R., Christensen, J., Cohen, M., Dastoor, A., Ilyin, I., Petersen, G., Syrakov, D., Artz, R., Davignon, D., Draxler, R., and Munthe, J. Intercomparison Study of Atmospheric Mercury Models. Phase II. Comparison of Models with Short-Term Measurements. Submitted to Atmospheric Environment.

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Conclu-sions


21





2000 European anthropogenic Hg emissions

240 t/yr



Conclu-sions


European anthropogenic Hg re-emissions

50 t/yr

European natural Hg emissions

180 t/yr



Conclu-sions


global natural Hg emissions1800 t/yr

1995 global anthropogenic Hg emissions1900 t/yr

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Conclu-sions


24

Phase III Sampling Locations



Conclu-sions


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Due to resource constraints, not all models simulated the entire year 1999…

EMAP

DEHM

MSCE-HEM

MSCE-HM

ADOM

HYSPLIT

CMAQ

DecNovOctSepAugJulJunMayAprMarFebJan



Conclu-sions


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There are uncertainties in measurements --even of precipitation amount…

NL91 De Zilk

020406080

100120140160

Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec

Months

Pre

cipi

tatio

n am

ount

, mm

HM samplerHg sampler

FI96 Pallas

0

20

40

60

80

100

120

Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec

Months

Pre

cipi

tatio

n am

ount

, mm

HM samplerHg sampler



Conclu-sions


DE01 DE09 NL91 NO99 SE02 SE11 SE12 SE05 FI96

Monitoring Station

0.0

0.5

1.0

1.5

wet

Hg

depo

sitio

n (g

/km

2-m

onth

)

Obs

MSCE-HM

MSCE-HM-Hem

HYSPLIT

DEHM

EMAP

ADOM

CMAQ

February 1999 Mercury Wet Deposition

27



Conclu-sions


28


Monitoring Station

0.0

0.5

1.0

1.5

2.0

2.5

3.0

wet

Hg

depo

sitio

n (g

/km

2-m

onth

)

Obs

MSCE-HM

MSCE-HM-Hem

HYSPLIT

DEHM

EMAP

CMAQ

August 1999 Mercury Wet Deposition



Conclu-sions


29


Monitoring Station

0.0

5.0

10.0

15.0

20.0

wet

Hg

depo

sitio

n (g

/km

2-ye

ar)

Obs

MSCE-HM

MSCE-HM-Hem

DEHM

EMAP

Full Year 1999 Mercury Wet Deposition



Conclu-sions


30

F2 F3 F5 F10Deviation Factor

0

20

40

60

80

100

Perc

ent o

f res

ults

with

in a

giv

en fa

ctor

ADOMCMAQEMAPMSCE-HMMSCE-HM-HemHYSPLITDEHM

Wet Deposition Summary

~60% within a factor of 2






Conclu-sions


31

For dry deposition, there are no measurement results to compare the models against;

However, the models can be compared against each other…



Conclu-sions


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Monitoring Station

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

Hg

dry

depo

sitio

n (g

/km

2-m

onth

)

model avg

MSCE-HM

MSCE-HEM

HYSPLIT

DEHM

EMAP

ADOM

CMAQ

February 1999 Mercury Dry Deposition



Conclu-sions


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Monitoring Station

0.00.10.20.30.40.50.60.70.8

Hg

dry

depo

sitio

n (g

/km

2-m

onth

)

model avg

MSCE-HM

MSCE-HEM

HYSPLIT

DEHM

EMAP

CMAQ

August 1999 Mercury Dry Deposition



Conclu-sions


34


Monitoring Station

0.0

1.0

2.0

3.0

4.0

5.0

6.0

7.0

Hg

dry

depo

sitio

n (g

/km

2-ye

ar)

model avg

MSCE-HM

MSCE-HEM

DEHM

EMAP

Full Year 1999 Mercury Dry Deposition



Conclu-sions


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In the following, the total model-predicted deposition (= wet + dry) is compared



Conclu-sions


36

February 1999

0

0.2

0.4

0.6

0.8

1

1.2

1.4

1.6

NL91 DE09 DE01 SE11 SE02 NO99 SE12 SE05 FI96

Stations from south to north

Tota

l Hg

depo

sitio

n,

g/km

2 /y

ADOMEMAPMSCE-HMMSCE_HM_HemHYSPLITDEHMCMAQ

Total Modeled Hg Deposition (wet + dry)



Conclu-sions


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Total Modeled Hg Deposition (wet + dry)August 1999

0

0.5

1

1.5

2

2.5

3

3.5



Tota

l Hg

depo

sitio

n,

g/km

2 /y

ADOMEMAPMSCE-HMMSCE-HM-HemHYSPLITDEHMCMAQ

Note: ADOM was not run for August, so for this graph, ADOM results for July were used



Conclu-sions


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Total Modeled Hg Deposition (wet + dry)1999 as whole

0

5

10

15

20



Tota

l Hg

depo

sitio

n,

g/km

2 /y

EMAPMSCE-HM

MSCE-HM-HemDEHM



Conclu-sions


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Main items of mercury atmospheric balance for the UK in 1999, t/yr



Conclu-sions


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Items of Hg atmospheric balances for the countries in 1999, t/yr[average modeled result (with ranges in parentheses)]

18.2(16–21)

8.4(7.9-9.2)

7.3 (7.0-7.8)

Outflow

2.1(1.4-2.6)

0.8(0.5-1.3)

0.3(0.2-0.6)

Dep. from European emissions

7.4(4.8-9.1)

1.3(0.6-1.9)

1.3 (0.8-1.6)

Dep. from own emissions

11.8(9.6-13.1)

4.7(3.2-6.6)

3.5(3.1-4.2)

Total deposition

PolandItalyThe UKItem



Conclu-sions


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11903342400.391.03Maximum

7301641700.190.65MSCE-HM-Hem

10702612350.160.54MSCE-HM

300143760.100.24Minimum

PolandItalyThe UKDryWet

Total deposition over the countries in Feb 1999, kg

Deposition over polluted area in Feb

1999, g/km2Range

EMEP model results in relation to the other models



Conclu-sions


42

Stage III Publication:

2005 Ryaboshapko, A., Artz, R., Bullock, R., Christensen, J., Cohen, M., Draxler, R., Ilyin, I., Munthe, J., Pacyna, J., Petersen, G., Syrakov, D., Travnikov, O. Intercomparison Study of Numerical Models for Long Range Atmospheric Transport of Mercury. Stage III. Comparison of Modelling Results with Long-Term Observations and Comparison of Calculated Items of Regional Balances. Meteorological Synthesizing Centre – East, Moscow, Russia.



Conclu-sions


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Conclusions: Uncertainties in Mercury Modeling

• Elemental Hg in air - factor of 1.2• Particulate Hg in air - factor of 1.5• Oxidized gaseous Hg in air - factor of 5• Total Hg in precipitation - factor of 1.5• Wet deposition - factor of 2.0• Dry deposition - factor of 2.5• Balances for countries - factor of 2



Conclu-sions


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Conclusions• Based on this Intercomparison Study, EMEP

operational models for mercury correspond to the most advanced scientific models in terms of formulation and with respect to the accuracy of modelling results;

• Based on this Intercomparision Study, EMEP operational models for mercury can provide useful, policy-relevant data in conjunction with the goals of the HM Protocol.



Conclu-sions


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Thanks!

All of the participants in the mercury modeling study are grateful to MSC-East for their leadership and collegiality throughout the project

The scientific community’s understanding of atmospheric mercury and models have benefited greatly from this project

EMEP Intercomparison Study of Numerical Models for Long ...Long-Range Atmospheric Transport of...

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