Sensitivity of PM 2.5 Species to Emissions in the Southeast Sun-Kyoung Park and Armistead G. Russell…

Sensitivity of PM 2.5 Species to Emissions in the Southeast

Sun-Kyoung Park and Armistead G. RussellGeorgia Institute of Technology

Sensitivity of PM 2.5 species to Emissions in the Southeast

OVERVIEW

Contents

• Model Domain• Meteorological Input • Input of SMOKE and Modules in CMAQ• CMAQ 4.2.2 vs. 4.3• Sensitivity of PM 2.5 to Emissions• Conclusion

• Comparison between CMAQ 4.2.2 and 4.3• Sensitivity of PM 2.5 to emissions in the Southeast for July 2001 and

January 2002 using Models-3 (CMAQ 4.3/MM5/SMOKE)


1. Model Domain14,500 m (=0.0)

7,200 m (=0.3)

70 m (=0.99)

2,940 m (=0.65)

1,550 m (=0.80)

740 m (=0.90)

300 m (=0.96)

140 m (=0.98)

18 m (=0.9975)

CMAQ horizontal domain and the vertical structure.


Model CMAQ MM5

Grid size 36 km 12 km 36 km 12 km

Dimension 147 x 111 21 x 18 164 x 128 27 x 24

Coordinate of the origin (-2,628, -1,980 km) (1,044, -720 km) (-2,952, -2,304 km) (1,008, -756 km)

Number of vertical layer 9 25

Top pressure of the model domain 100 hPa 100 hPa

2. Meteorological Input

MM5 version 3.5.3:Simple ice microphysicsKain-Fritsch cumulus scheme Rapid radiative transfer modelPleim Chang planetary boundary layerPleim-Xiu land surface model

Four Dimensional Data Assimilation:

NCEP Eta model outputs for the GCIP project NCEP ADP Observational data

Evaluation:

TDL surface hourly data

Temperature(K)

SpecificHumidity

(g/kg)

WindSpeed

(m/sec)

WindDirection

(deg)

MBEJuly 2001(36 km) -0.333 -0.82 -0.092 11.59

July 2001(12 km) 0.2 -0.504 0.148 35.7

January 2002(36 km) -1.161 0.101 0.135 21.62

January 2002(12 km) -1.34 0.051 0.011 8.64

RMSEJuly 2001(36 km) 1.65 1.806 1.297 58.05

July 2001(12 km) 1.998 1.156 1.41 78.72

January 2002(36 km) 2.053 0.524 1.412 64.6

January 2002(12 km) 2.48 0.396 1.629 54.18




Temperature (K) Specific Humidity (g/kg) Wind Speed (m/sec)July 2001

January 2002

RMSE

Temperature

0

0.5

1

1.5

2

2.5

3

July2001

(36 km)

July2001

(12 km)

January2002

(36 km)

January2002

(12 km)

K

Wind Speed

0

0.5

1

1.5

2

2.5

July2001

(36 km)

July2001

(12 km)

January2002

(36 km)

January2002

(12 km)

m/s

ec

Specific Humidity

0

0.5

1

1.5

2

2.5

July2001

(36 km)

July2001

(12 km)

January2002

(36 km)

January2002

(12 km)

g/kg

Statistical benchmark (Emery et al., (2001))

Emery, C., E. Tai and G. Yarwood, 2001. “Enhanced meteorological modeling and performance evaluation for two Texas episodes”, report to the Texas National Reesources Conservation Commision, prepared by ENVIRON, International Corp, Novato, CA



3. Input of SMOKE and Modules in CMAQ

• Input of SMOKE

• Emissions inventory developed by GA Tech for the state of Georgia and 1999 National emissions inventory for other states

• EGAS 4.0 growth factors and existing control strategy to project the 1999 emissions to 2001 and 2002 emissions

• Modules in CMAQ

• Chemical mechanism: SAPRC-99

• Chemistry solver: modified Euler backward iterative (MEBI) method

• Cloud: the regional acid deposition model (RADM)

• Aerosol dynamics: AERO3

• Deposition velocities of aerosols: AERO_DEPV2

• Horizontal and vertical advection: piecewise parabolic method (PPM)

• Minimum vertical eddy coefficient: 0.3 m2/sec.



0

5

10

15

20

25

30

MODEL (July 2001) OBS (July 2001) MODEL (January2002)

OBS (January 2002)

SULFATE(ug/m3) NITRATE(ug/m3) AMMONIUM(ug/m3) EC(ug/m3) OC(ug/m3) Others

YRK station

0

5

10

15

20

25

30

35

MODEL(July2001)

OBS(July2001)

MODEL(January

2002)

OBS(January

2002)ug

/m3

BHM station

0

5

10

15

20

25

30

35

MODEL(July2001)

OBS(July2001)

MODEL(January

2002)

OBS(January

2002)

ug/m

3

4. CMAQ 4.2.2 vs. 4.3 (daily PM 2.5)The performance of CMAQ was evaluated with measured data of SEARCH and ASACA stations

JST

0

1

2

3

4

5

6

7

0 2 4 6

OBS (ug/m3)

MO

DEL

(ug/

m3)

4. CMAQ 4.2.2 vs. 4.3 (daily PM 2.5, July 2001)

• 36 km (version 4.2.2) • 36 km (version 4.3) • 12 km (version 4.2.2) • 12 km (version 4.3)

Sulfate AmmoniumNitrate

PM 2.5Organic Carbon

Elemental Carbon

OBS x 2

OBS x 0.5


0

2

4

6

8

10

12

14

0 2 4 6 8 10 12 14

OBS (ug/m3)

MO

DEL

(ug/

m3)

0

0.5

1

1.5

0 0.5 1 1.5

OBS (ug/m3)M

OD

EL (u

g/m

3)

0

1

2

3

0 1 2 3

OBS (ug/m3)

MO

DEL

(ug/

m3)

0

5

10

15

20

0 5 10 15 20

OBS (ug/m3)

MO

DEL

(ug/

m3)

0

10

20

30

40

0 10 20 30 40

OBS-TEOM (ug/m3)

MO

DEL

(ug/

m3)

0

1

2

3

0 1 2 3

OBS (ug/m3)

MO

DEL

(ug/

m3)

4. CMAQ 4.2.2 vs. 4.3 (daily PM 2.5, January 2002)

Sulfate Nitrate Ammonium

Elemental Carbon

Organic Carbon PM 2.5

OBS x 2

OBS x 0.5



0

1

2

3

4

5

0 1 2 3 4 5

OBS (ug/m3)

MO

DEL

(ug/

m3)

0

1

2

3

4

0 1 2 3 4

OBS (ug/m3)M

OD

EL (u

g/m

3)

0

1

2

3

4

5

0 1 2 3 4 5

OBS (ug/m3)

MO

DEL

(ug/

m3)

0

5

10

15

20

0 5 10 15 20

OBS (ug/m3)

MO

DEL

(ug/

m3)

0

5

10

15

20

25

0 10 20

OBS-TEOM (ug/m3)M

OD

EL (u

g/m

3)

0

500

1000

1500

2000

0 500 1000 1500 2000

OBS (ppb)

MO

DEL

(ppb

)

4. CMAQ 4.2.2 vs. 4.3 (hourly gas phase species, July 2001)

CO

HNO3NOy PM 2.5

O3 MBE (ppb)

MNB (%)

MGE (ppb)

MNGE (%)

Version 4.2.2

5.38 13.7 24.83 44.35

Version 4.3

11.16 21.6 20.24 38.1

Statistics of O3 (12 km domain)O3

OBS x 2

OBS x 0.5



0

50

100

150

0 50 100 150

OBS (ppb)

MO

DEL

(ppb

)

0

50

100

150

200

0 50 100 150 200

OBS (ppb)

MO

DEL

(ppb

)

0

1

2

3

4

5

6

0 1 2 3 4 5 6

OBS (ppb)

MO

DEL

(ppb

)

0

20

40

60

80

100

0 20 40 60 80 100

OBS (ug/m3)M

OD

EL (u

g/m

3)

Performance of CMAQ for PM 2.5 species

• Sulfate: overestimated in July 2001 good in January 2002

• Nitrate: overestimated

• Ammonium: good

• Elemental Carbon: overestimated

• Organic carbon: from version 4.2.2 to 4.3, the performance is improved markedly after the secondary organic aerosol algorithm has been modified to make the gas-particle partitioning of semi-volatiles reversible

• PM 2.5: overestimated mainly due to the overestimation of the crustal elements (primary PM 2.5)


4. CMAQ 4.2.2 vs. 4.3 (hourly gas phase species, July 2001)

5. Sensitivity of PM 2.5 to Emissions

Sulfate: Major species of the PM 2.5 in the Southeast. Sources: anthropogenic emissions

Sensitivity of emissions to sulfate sensitivity of emissions to PM 2.5

• 20% reduction of SO2

• 20% reduction of NH3

• 20% reduction of NH3 and SO2


-18

-12

-6

0sens

itivi

ty (%

)

0

5

10

15

conc

entr

atio

n (u

g/m

3)

-18

-12

-6

0sens

itivi

ty (%

)

0

5

10

15co

ncen

trat

ion

(ug/

m3)

Sulfate Nitrate

0

20

40

60sens

itivi

ty (%

)

0

5

10

conc

entr

atio

n (u

g/m

3)

0

20

40

60sens

itivi

ty (%

)

0

5

10

conc

entr

atio

n (u

g/m

3)

July 2001

January 2002

5. Sensitivity of PM 2.5 to Emissions (20% reduction of SO2)


: sensitivity, •: concentration

-10

-5

0sens

itivi

ty (%

)

0

2

4

conc

entr

atio

n (u

g/m

3)

-10

-5

0sens

itivi

ty (%

)

0

2

4co

ncen

trat

ion

(ug/

m3)

Ammonium PM 2.5

July 2001

January 2002

5. Sensitivity of PM 2.5 to Emissions (20% reduction of SO2)



-2

-1

0GFP

OAKOLE CTR

PNSBHM

YRKFTM

JST

SDKTUCD

mas

s (u

g/m

3)

0

30

60

conc

entra

tion

(ug/

m3)

-2

-1

0GFP

OAKOLE CTR

PNSBHM

YRKFTM

JST

SDKTUCD

mas

s (u

g/m

3)

0

30

60

conc

entra

tion

(ug/

m3)

D mass

Sulfate Nitrate

5. Sensitivity of PM 2.5 to Emissions (20% reduction of NH3)

-6

-3

0 GFP

OA

K

OLE

CTR

PNS

BH

MYR

K

FTM

JST

SDK

TUC

sen

sitiv

ity (%

)

0

5

10

15

conc

entr

atio

n (u

g/m

3)

-6

-3

0 GFP

OA

K

OLE

CTR

PNS

BH

M

YRK

FTM

JST

SDK

TUC

sens

itivi

ty (%

)

0

5

10

15co

ncen

trat

ion

(ug/

m3)

July 2001

January 2002

-60

-40

-20

0 GFP

OA

KO

LEC

TRPN

S

BH

MYR

KFTMJSTSD

KTU

C

sens

itivi

ty (%

)

0

5

10

conc

entr

atio

n (u

g/m

3)

-60

-40

-20

0 GFP

OA

K

OLE

CTR

PNS

BH

M

YRK

FTM

JST

SDK

TUC

sens

itivi

ty (%

)

0

5

10

conc

entr

atio

n (u

g/m

3)

: sensitivity, •: concentrationSensitivity of PM 2.5 species to Emissions in the Southeast

5. Sensitivity of PM 2.5 to Emissions (20% reduction of NH3) PM 2.5Ammonium

July 2001-20

-10

0 GFP

OA

K

OLE

CTR

PNS

BH

M

YRK

FTM

JST

SDK

TUC

sens

itivi

ty (%

)

0

2

4

conc

entr

atio

n (u

g/m

3)

-20

-10

0 GFP

OA

K

OLE

CTR

PNS

BH

M

YRK

FTM

JST

SDK

TUC

sens

itivi

ty (%

)

0

2

4

conc

entr

atio

n (u

g/m

3)



-2

-1

0 GFP

OA

KO

LEC

TRPN

SB

HM

YRK

FTMJSTSD

KTU

C

D m

ass

(ug/

m3)

0

30

60

conc

entra

tion

(ug/

m3)

-2

-1

0 GFP

OA

KO

LEC

TRPN

S

BH

MYR

KFTMJSTSD

KTU

C

D m

ass

(ug/

m3)

0

30

60

conc

entra

tion

(ug/

m3)

D mass

January 2002

Sulfate NitrateJuly 2001

January 2002

-18

-12

-6

0 GFP

OA

K

OLE

CTR

PNS

BH

MYR

KFTMJST

SDK

TUC

sens

itivi

ty (%

)

0

5

10

15

conc

entr

atio

n (u

g/m

3)

-18

-12

-6

0 GFP

OA

KO

LEC

TR

PNS

BH

MYR

K

FTMJSTSD

K

TUC

sens

itivi

ty (%

)

0

5

10

15

conc

entr

atio

n (u

g/m

3)

-40

-20

0 GFP

OA

KO

LEC

TR

PNS

BH

MYR

K

FTMJSTSD

K

TUC

sens

itivi

ty (%

)

0

5

10

conc

entr

atio

n (u

g/m

3)

-40

-20

0 GFP

OA

KO

LEC

TR

PNS

BH

MYR

K

FTMJSTSD

K

TUC

sens

itivi

ty (%

)

0

5

10

conc

entr

atio

n (u

g/m

3)

5. Sensitivity of PM 2.5 to Emissions (20% reduction of NH3 and SO2)



Ammonium PM 2.5July 2001

-30

-20

-10

0 GFP

OA

K

OLE

CTR

PNS

BH

M

YRK

FTM

JST

SDK

TUC

sens

itivi

ty (%

)

0

2

4

conc

entr

atio

n (u

g/m

3)

-30

-20

-10

0 GFP

OA

K

OLE

CTR

PNS

BH

M

YRK

FTM

JST

SDK

TUC

sens

itivi

ty (%

)

0

2

4

conc

entr

atio

n (u

g/m

3)

5. Sensitivity of PM 2.5 to Emissions (20% reduction of NH3 and SO2)



-3

-2

-1

0 GFP

OA

KO

LEC

TRPN

S

BH

MYR

KFTMJSTSD

KTU

C

D m

ass

(ug/

m3)

0

30

60

conc

entra

tion

(ug/

m3)

-3

-2

-1

0 GFP

OA

KO

LEC

TRPN

SB

HM

YRK

FTMJSTSD

KTU

C

D m

ass

(ug/

m3)

0

30

60

con

cent

ratio

n (u

g/m

3)

D mass

January 2002



-5

0

5

10

15

20

25

30

BASE SO2_20 NH3_20 NH3_SO2_20

SULFATE(ug/m3) NITRATE(ug/m3) AMMONIUM(ug/m3) EC(ug/m3) OC(ug/m3) Others(ug/m3)

Yorkville (January 2002)

-5

0

5

10

15

20

25

30

BA

SE

SO

2_20

NH

3_20

NH

3_SO

2_20

ug/m

3

Tucker (July 2001)

-5

0

5

10

15

20

25

30

35

40

45

BA

SE

SO

2_20

NH

3_20

NH

3_SO

2_20

ug/m

3

Tucker (January 2002)

-5

0

5

10

15

20

25

30

35

40

45B

AS

E

SO

2_20

NH

3_20

NH

3_SO

2_20

ug/m

3

Yorkville (July 2001)

-5

0

5

10

15

20

25

30

BA

SE

SO

2_20

NH

3_20

NH

3_SO

2_20

ug/m

3

• The sensitivity of PM 2.5 to a 20% reduction of NH3: high in January 2002 SO2: high in July 2001 NH3 and SO2: high in both January 2002 and July 2001

20 % of SO2 20 % of NH3 20 % of NH3 and SO2

July 2001

-6.0 % ( -1.61 g/m3)

-2.19 % (-0.59 g/m3)

-8.01 % (-2.15 g/m3)

January 2002

-0.96 % (-0.26 g/m3)

-5.62 % (-1.53 g/m3)

-6.4 % (-1.74 g/m3)



6. Summary• CMAQ 4.3 improved markedly in simulation of organic carbon concentration. However, model still overestimates primary PM 2.5 species.

• When SO2 is reduced, sulfate concentrations decreased, but nitrate concentrations increased. Thus, only SO2 reduction was not efficient way to reduce the PM 2.5 in winter time, when the nitrate concentrations are relatively high.

• When NH3 is reduced, nitrate and ammonium decreased, but sulfate concentrations did not change much. Thus, NH3 reduction did not decrease PM 2.5 in summer time, when the sulfate concentrations are relatively high.

• When NH3 and SO2 are both reduced, nitrate, sulfate and ammonium concentrations decreased significantly both summer and winter.

• Future research will include the sensitivity of emissions for different geographic locations.


Documents

Sensitivity of PM 2.5 Species to Emissions in the Southeast Sun-Kyoung Park and Armistead G. Russell…