source apportionment of pm 2.5 in the southeastern us sangil lee 1, yongtao hu 1, michael chang 2,...

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Source Apportionment of PM2.5 in the Southeastern US

Sangil Lee1, Yongtao Hu1, Michael Chang2,Karsten Baumann2, Armistead (Ted) Russell1

1School of Civil and Environmental Engineering 2School of Earth and Atmospheric Sciences Georgia Institute of Technology, Atlanta, GA

Concerns

• Adverse Health Effects PM mass, chemical composition (sulfate, EC,

OC etc), size

• Identify PM sources • Understand a relationship between sources and

adverse health effects

• Develop control strategies of PM

EPA STN sites

• PM2.5 chemical composition (ionic species, OC & EC, trace elements)− covers from January 2002 to November 2003

Rome

Macon

Athens

Mobile

Douglas

AtlantaAugusta

Memphis

Decatur

SavannahColumbus

Columbia

Pensacola

Kingsport

Nashville

Greenville

CharlestonMontgomery

Birmingham

Tallahassee

Chattanooga

Chesterfield

Lawrenceburg

every 3 dayevery 6 day

y = 2.8x + 1.5

R2 = 0.97

y = 2.6x + 0.5

R2 = 0.95

y = 2.7x + 0.4

R2 = 0.98y = 2.9x

R2 = 0.970

2

4

6

8

10

12

14

0 1 2 3 4

EC, mg/m3

OC

, mg

/m3

All January July

Primary and Secondary OC

30%

5%

9%33%

6%

3%

14%

Sulfate

Nitrate

Ammonium

OC

EC

Trace Elements

UnIden

Atlanta, GA

SOC = OC - (OC/EC)primary x EC

SOC = OC - POCSignificant Uncertainty !

POC + SOC

Minimum OC/EC ratio approach (Castro et al., 1999)

SOC and ( Unidentified Mass+OC)/OC

0

20

40

60

80

100

Jan_

Feb

Mar

_May

June

_Aug

Sept_

Nov

Dec_F

eb

Mar

_May

June

_Aug

Sept_

Nov

SO

C /

OC

x10

0, %

1.0

1.2

1.4

1.6

1.8

2.0

2.2

(Un

i M

ass

+ O

C)/

OC

Atlanta, GA44 % SOC (20 % ~ 75 %) at Atlanta, August, 1999 (Lim and Turpin, 2002)

• seasonal variability of SOC• positive relationship between SOC and (Uni Mass + OC)/OC

max & minaveragestd

Primary OC/EC Ratios

Rome

Macon

Athens

Mobile

Douglas

AtlantaAugusta

Memphis

Decatur

Savannah

Columbus

Columbia

Pensacola

Kingsport

Nashville

Greenville

Charleston

Montgomery

Birmingham

Tallahassee

Chattanooga

Chesterfield

Lawrenceburg

6.3

4.1

5.5

3.9

4.1

6.0

2.9

5.5

6.4

3.34.7

4.1

6.2

4.8

3.5

2.9 4.4

4.2

3.6

4.25

3.5

4.4

3.6

2.5

Lower: major cities (more diesel vehicles) Higher: others (more biomass burning)

Source Apportionment- CMB Receptor Model -

m

jjjii SfC

1,

Ci : ambient concentration of species ifi,j : fraction of species i in source jSj : source contribution of source j

Wood burning: Fine et al. (2002)Motor vehicles: Schauer et al. (1999, 2002)Coal power plant: Chow et al. (2004)Dust, Pulp & Paper, Oil combustion,Metal, Mineral production: EPA SPECIATE 3.2

Source Apportionments

Rome

Macon

Athens

Mobile

Douglas

AtlantaAugusta

Memphis

Decatur

SavannahColumbus

Columbia

Pensacola

KingsportNashville

Greenville

Charleston

Montgomery

Birmingham

Tallahassee

Chattanooga

Chesterfield

Lawrenceburg

9.6

NH4HSO4

(NH4)2SO4

NH4NO3

SOC

Wood Burning

Motor Vehicles

Dust

Pulp, Paper

Coal

Mineral

Oil combustion

Metal

UnIden

Interpolation- Inverse Distance Weighted -

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20

12

mg/m3

PM2.5 mass

Interpolation- Inverse Distance Weighted -

NH4HSO4 (NH4)2SO4

NH4NO3 SOC

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4.2

0.5

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mg/m3

Interpolation- Inverse Distance Weighted -

Wood Burning Motor Vehicles

Coal Power Plant Pulp & Paper

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4.5

0.5

mg/m3

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1.5

0

mg/m3

Interpolation- Inverse Distance Weighted -

Dust Mineral Production

Oil Combustion Metal Production

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mg/m3

Port Shipping (?)

Comparisons with Emission InventoriesSource apportionment Emission

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mg/m3

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4.5

0.5

mg/m3

PM2.5

Motor VehiclesMax: 628 tons/yr

Max: 12,465 tons/yr

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mg/m3

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1.5

0

mg/m3

Mineral production

Pulp & Paper production

Comparisons with Emission InventoriesSource apportionment Emission

Max: 1,843 tons/yr

Max: 1,431 tons/yr

Spatial Correlations of Sources

• Which sources are/are not correlated in the region?

• Source correlation calculations– Pearson numbers between two sites were calculated for

each source based on daily source apportionment results– how daily source correlations are changed with distance

Spatial Correlations

PM2.5 mass

1.0

0.8

0.6

0.4

0.2

0.0

Pe

ars

on

No

.

10008006004002000

Distance (km)

y = exp(-0.0017x)

2= 4.29

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pe

ars

on

No

.

10008006004002000

Distance (km)

y = exp(-0.0020x)

NH4HSO4 + (NH4)2SO4

2= 6.31

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000Distance (km)

y = exp(-0.0025x)

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000

Distance (km)

y = exp(-0.0027x)

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000Distance (km)

y = exp(-0.0015x)

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000Distance (km)

y = exp(-0.0025x)

Spatial Source Correlations

NH4HSO4 (NH4)2SO4

NH4NO3 SOC

2= 8.00 2= 7.72

2= 6.27

2= 7.83

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000Distance (km)

y = exp(-0.0029x)

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000

Distance (km)

y = exp(-0.0033x)

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000

Distance (km)

y = exp(-0.0018x)

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000

Distance (km)

y = exp(-0.0045x)

Spatial Source Correlations

Wood Burning Motor Vehicles

Dust Pulp & Paper production

2= 9.64 2= 11.47

2= 19.70

2= 9.72

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000

Distance (km)

y = exp(-0.0056x)

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000

Distance (km)

y = exp(-0.0099x)

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000

Distance (km)

y = exp(-0.0103x)

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

Pea

rso

n N

o.

10008006004002000

Distance (km)

y = exp(-0.0053x)

Spatial Source Correlations

Coal Power Plant

Mineral Production

Oil Combustion

Metal Production

2= 9.32

2= 11.582= 7.95

2= 7.02

Summary• SOC : 40 ~ 60 % of OC, Seasonal difference

• Secondary PM : more than 50 % of PM

• Significant spatial variability of source contributions

• Agreement or disagreement with emission inventories

• Significant regional correlation; secondary PM, wood burning, motor vehicles, dust

• Little regional correlation; industrial sources

• Can identify port shipping impacts?

Acknowledgements

• Funding Agencies– U.S. EPA (RD82897602, RD83107601, and

RD83096001)– GA DNR– Georgia Power

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