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DEVELOPMENT AND APPLICATION OF MADRID: A NEW AEROSOL MODULE IN MODELS-3/CMAQ
Yang Zhang*, Betty Pun, Krish Vijayaraghavan, Shiang-Yuh Wu and Christian SeigneurAtmospheric and Environmental Research, Inc., San Ramon, CA
Spyros N. PandisCarnegie-Mellon University, Pittsburgh, PA
Mark Z. JacobsonStanford University, Stanford, CA
Athanasios NenesGeorgia Institute of Technology, Atlanta, GA
John H. SeinfeldCalifornia Institute of Technology, Pasadena, CA
EPA Models-3/CMAQ Workshop, October 27-29, 2003
* Current address: North Carolina State University
Presentation Outline
• Background– Development of CMAQ-MADRID
– CMAQ vs. CMAQ-MADRID
• 3-D Application– Application for SCAQS Episode
– Sensitivity Study
– Performance Evaluation
• Summary
Development of CMAQ-MADRID
• Model for Aerosol Dynamics, Reaction, Ionization, and Dissolution– Review of thermodynamic modules
– Review of aerosol dynamics modules
– Selection and integration of the modules
• 3-D Host Model - EPA Models-3/CMAQ– Evaluation of 3-D models (SAQM, MAQSIP, CMAQ, and CAMx)
– Selection protocol (sciences, computation, ease-of-use, modularity, documentation, technical support and community status)
• Incorporation of MADRID and CMU Aqueous Module into CMAQ– Preserves features of EPA Models-3/CMAQ
– Advanced aerosol and cloud modules
– Provided to EPA in December 2002
CMAQ vs. CMAQ-MADRID: PM Treatment
Models-3/CMAQ• Size representation Modal (3 modes)
• Inorganic species NH4+, SO4
=, NO3-, Na+, Cl-
• Equilibrium MARS-A, ISORROPIA
• Coagulation Modal approach
• Nucleation Absolute rate
• Condensation Modal approach
• Mass transfer Full equilibrium
• Dry deposition Resistance transfer
• SOA formation Irreversible absorption (6 precursors) (Pandis et al., 1992)
or reversible absorption (6 precursors) (Schell et al., 2001)
CMAQ-MADRID
Sectional (2 or multiple sections)
NH4+, SO4
=, NO3-, Na+, Cl-
ISORROPIA
Not treated
Relative rate
Moving-center approach
CIT equilibrium and CMU hybrid
Revised flux approach
MADRID 1: Absorption (38 species)
(Odum et al., 1997; Griffin et al., 1999)
MADRID 2: Absorption & dissolution
(42 VOCs, 5 hydrophobic and 5
hydrophilic surrogate SOA)
(Pun et al., 2002)
CMAQ vs. CMAQ-MADRID: Chemical Mechanisms
Models-3/CMAQ
• Gas-phase CBM-IV, RADM2, chemistry SAPRC-99(1)
• Aqueous RADM
chemistry (Walcek and Taylor, 1986)
- 33 aqueous/ionic species
- 18 equilibria
- 5 kinetic reactions
- 55 species for wet deposition
• Heterogeneous Not treatedchemistry
CMAQ-MADRID
CBM-IV/RADM2 (MADRID 1)
CACM (MADRID 2)
CMU
(Seinfeld and Pandis, 1998)
- 55 aqueous/ionic species
- 34 equilibria
- 99 kinetic reactions
- 88 species for wet deposition
HO2, NO2, NO3, N2O5 on PM N2O5 in droplet (Jacob, 2000)
(1) available in July 2002 version of Models-3/CMAQ
Application of CMAQ-MADRID: SCAQS 1987 Episode
• Period 25-29 August 1987• Domain 63 x 28 grid cells• Horizontal resolution 5 km• Vertical resolution 15 layers• Meteorology
– MM5/FDDA– Nested grids (45, 15, 5 km)
• Emissions– NOx, SO2, CO, SO3, VOC
(Allen and Wagner, 1992)– NH3 and PM (Meng et al., 1998)
– Adjustment in VOC (Pai et al., 2000)• Initial and boundary conditions
– Gases (Pai et al., 2000)– PM (San Nicholas Island)
SCAQS Modeling Domain and Ozone/PM Measurement Sites
▲- sites with PM (5 samples/day) and ozone (hourly) measurements - sites with ozone (hourly) measurementsPink/Red - sites with ozone time series plotsBlue/Red - sites with 24-hr average PM concentrations/size distribution plots
ANAH
AZUSBURK
CELACLAR
HAWT
LBCC
RIVR
CRESELRI
POMAWSLA
BANN
COST
FONT
GLEN
HEMEINDOLGBH
LSAL
LYNN
NEWL
NORC
OJAI
PASA
PERI
PICO
PLSP
RDLD
SIMI
SNBOUPLA
VCTC
VENT
WHIT
HESP
RESE
PIRU
THSO
Observed vs. Simulated Ozone Mixing Ratios
POMA, central, rural
0
50
100
150
200
250
300
0 4 8 12 16 20 24 28 32 36 40 44 48Time (Hours from 0000PST August 27, 1987)
[O3
], p
pb
CELA, western, urban
0
50
100
150
200
250
300
0 4 8 12 16 20 24 28 32 36 40 44 48Time (Hours from 0000PST August 27, 1987)
[O3
], p
pb
RIVR, inland, urban
0
50
100
150
200
250
300
0 4 8 12 16 20 24 28 32 36 40 44 48Time (Hours from 0000PST August 27, 1987)
[O3
], p
pb
WSLA, watern, near coast
0
50
100
150
200
250
300
0 4 8 12 16 20 24 28 32 36 40 44 48Time (Hours from 0000PST August 27, 1987)
[O3
], p
pb
ELRI, northwestern, rural
0
50
100
150
200
250
300
0 4 8 12 16 20 24 28 32 36 40 44 48Time (Hours from 0000PST August 27, 1987)
[O3
], p
pb
CRES, northern, remote
0
50
100
150
200
250
300
0 4 8 12 16 20 24 28 32 36 40 44 48Time (Hours from 0000PST August 27, 1987)
[O3
], p
pb
Observed vs. Simulated PM2.5 Concentrations
24 hr-Avg. PM2.5 at HAWT, Aug. 27, 1987
0
5
10
15
20
25
30
35
PM Species
Mass c
on
c.,
g m
-3 Observed
CMAQ-MADRID 1
Na+ SO4= NH4+ NO3- OMCl- EC PM2.5
24 hr-Avg. PM2.5 at HAWT, Aug. 28, 1987
0
5
10
15
20
25
30
35
PM Species
Mass c
on
c.,
g m
-3 Observed
CMAQ-MADRID 1
Na+ SO4= NH4+ NO3- OMCl- EC PM2.5
24 hr-Avg. PM2.5 at CELA, Aug. 27, 1987
0
10
20
30
40
50
60
PM Species
Mass c
on
c.,
g m
-3
Observed
CMAQ-MADRID 1
Na+ SO4= NH4+ NO3- OMCl- EC PM2.5
24 hr-Avg. PM2.5 at CELA, Aug. 28, 1987
0
10
20
30
40
50
60
PM Species
Mass c
on
c.,
g m
-3
Observed
CMAQ-MADRID 1
Na+ SO4= NH4+ NO3- OMCl- EC PM2.5
24 hr-Avg. PM2.5 at RIVR, Aug. 27, 1987
0
20
40
60
80
100
PM Species
Mass c
on
c.,
g m
-3 Observed
CMAQ-MADRID 1
Na+ SO4= NH4+ NO3- OMCl- EC PM2.5
24 hr-Avg. PM2.5 at RIVR, Aug. 28, 1987
0
20
40
60
80
100
PM Species
Mass c
on
c.,
g m
-3 Observed
CMAQ-MADRID 1
Na+ SO4= NH4+ NO3- OMCl- EC PM2.5
MADRID 1 vs. MADRID 2 (Riverside)
28-August
27-August
Observed MADRID 1 MADRID 2
Nitrate OC
Sulfate EC
Ammonium Other
42%
9%13%
15%
4%
17%
37%
13%16%
9%
2%
23%
42%
10%13%
16%
4%
15%
42%
11%17%
8%
2%
20%
36%
13%16%
13%
2%
20%
33%
14%15%
14%
2%
22%
Condensational Growth (Moving-Center vs. Finite-Difference)
CLAR, 24-hr Average, August 28, 1987
0
20
40
60
80
0.01 0.1 1 10
Particle Diameter, Dp (m)
dM/d
log
Dp
(g
m-3
)
Observed
Moving-Center
Finite-Difference
RIVR, 24-hr Average, August 28, 1987
0
20
40
60
80
100
0.01 0.1 1 10
Particle Diameter, Dp (m)
dM/d
log
Dp
(g
m-3
)
Observed
Moving-Center
Finite-Difference
Gas/Particle Mass Transfer (Hybrid vs. Bulk Equilibrium)
CLAR, 24-hr Average, August 28, 1987
0
10
20
30
40
50
60
0.01 0.1 1 10
Particle Diameter, Dp (m)
dM/d
log
Dp
(
g m
-3)
ObservedCMU hybridCIT bulk equilibriumSimple bulk equilibrium
RIVR, 24-hr Average, August 28, 1987
0
20
40
60
80
100
0.01 0.1 1 10
Particle Diameter, Dp (m)
dM/d
log
Dp
(
g m
-3)
ObservedCMU hybridCIT bulk equilibriumSimple bulk equilibrium
Gas/Particle Mass Transfer (CIT Bulk Equilibrium vs. CMU Hybrid)
The CMU hybrid approach predicts more sodium nitrate in the coarse mode
The CIT bulk equilibrium approach distributes most nitrate within the fine mode (PM2.5)
HAWT, 24-hr Avg., Aug. 28, 1987, CMU Hybrid Approach
0
1
2
3
4
1 2 3 4 5 6 7 8
SectionCo
ncen
tratio
ns,
g m
-3 Cl-NO3-NH4+SO4=Na+
HAWT, 24-hr Avg, Aug. 28, 1987, CIT Hybrid Approach
0
1
2
3
4
1 2 3 4 5 6 7 8
Section
Conc
entra
tions
, g
m-3 Cl-
NO3-NH4+SO4=Na+
Model Performance for O3 and PM2.5
August 27-28 Other work* Gross
error,% Bias %
Gross error, %
Bias, %
O3 33.6 8.5 -35 to 50 -6.6 to 34 PM2.5 44.2 14.2 32 to 66 -26 to 46 Sulfate2.5 37.9 11 28.4 to 49 -47 to 3.7 Nitrate2.5 44.2 -37.8 29 to 187 -20.7 to 106 Ammonium2.5 52.3 25.3 18 to 67.8 -52.3 to 56 EC2.5 54.1 -20.2 15 to 77 -52 to 35 OM2.5 49.6 -21.3 38 to 126 -44.1 to 112
* Other work include UAM-IV/CALGRID/UAM-AERO (Kumar et al., 1994; Lurmann et al., 1997), GATOR (Jacobson, 1997), SMOG (Lu et al., 1997), CIT with SAPRC93 or LCC (Harley et al., 1993, 1997; Meng et al., 1998), SAQM-AERO (Pai et al., 2000).
Summary of SCAQS Application
• CMAQ-MADRID provides a realistic representation of atmospheric PM.
• Secondary organic aerosol predictions are sensitive to different SOA formulations.
• Jacobson’s moving-center approach is the most accurate among the condensational growth algorithms tested.
• The CMU hybrid and the CIT bulk equilibrium approaches predict a realistic particle size distribution under most conditions.
• Heterogeneous chemistry increases H2O2, HNO3, and sulfate; decreases SO2 and NO2; affects O3 and nitrate in both ways.
Acknowledgments
• EPRI: New aerosol & cloud modules• CARB: MADRID2 aerosol module• R. Griffin and D. Dabdub for providing source
codes used in MADRID• F. Binkowski and S. Leduc for discussions
regarding EPA Models-3/CAMQ• Project managers: N. Kumar (EPRI), A. Hansen
(EPRI), N. Motallebi (CARB)