k. baumann, m.h. bergin, w.l. chameides, f. ift, c.s. kiang, j.z. zhao
DESCRIPTION
Fine Particle (PM 2.5 ) Composition and Trace Gas Measurements in the Yangtze Delta Region In memoriam Dr. Glen Cass. K. Baumann, M.H. Bergin, W.L. Chameides, F. Ift, C.S. Kiang, J.Z. Zhao School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta - PowerPoint PPT PresentationTRANSCRIPT
Fine Particle (PM2.5) Composition and Trace Gas Measurements in the Yangtze Delta Region
In memoriam Dr. Glen Cass
K. Baumann, M.H. Bergin, W.L. Chameides, F. Ift, C.S. Kiang, J.Z. Zhao
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta
K.S. Shao, X.Y. Tang, M.L. Wang, L.M. Zeng
Center for Environmental Sciences, Peking University, Beijing
Locations, tools, and data quality
Meteorological and trace gas characteristics at SheShan
Spatial trends in PM2.5 mass and composition
Seasonal comparison based on ChangShu data
2
Sampling Locations in the Yangtze Delta
3
Sampling Locations in the Yangtze Delta
SheShanLinAn
4
Continuous Trace Gas Measurements
Yangtse network station set-up
The inlet box, mounted on the roof of the SheShan observatory, allowed standard addition of NO, and NO2 (via GPT) calibration
gases. A single chemiluminescence detector was utilized, alternating between NO and NOy measure modes every 2 min with instrument zeroes overlapping every 15 min. The flow controller stream selector valve assembly was housed inside
resulting in a sample residence time of ~7 s. The NOy converter is a 35 cm long, 0.48 cm ID MoO tube, temperature controlled
at 330 ±2 oC. All air intake surfaces were Teflon coated and T-controlled at 40 oC.
SheShan Nov-99 intensive NO/NOy
5
Discrete PMfine Measurements via Particle Composition Monitor (PCM)
6
PCM Data Quality
Ca2+ Na+ K+ NH4+ Cl- NO3
- SO42- Acet Form Oxal OC EC
DL (ug m-3) 0.03 0.50 0.16 0.07 0.49 0.43 0.13 0.56 0.42 0.00 0.91 0.51
Bias (%) 60 56 20 30 15 21 17 53 186 34 11 33
STD (%) 30 39 22 18 11 15 13 41 39 30 7 25
7
Trace Gas Data Quality
NO NOy O3 SO2
DL (ppbv) 0.003 0.3 1 1
Precision (%) ± 10 ± 15 ± 2 ± 5
Accuracy (%) ± 10 ± 25 ± 2 ± 5
Note: values for NO/NOy are from GIT’s research grade analyzer, and
uncertainty in NOy arises from MoO conversion efficiency determined for NO2 Q(NO2) = 67 ±14 %.
8
Average PM2.5 and PM10 Concentrationsfor SheShan November 99
PM2.5 (ug m-3) PM10 (ug m-3) PM2.5/PM10
Na+ 0.31 ±0.12 0.89 ±0.43 0.41 ±0.21
K+ 2.19 ±1.41 n/a n/a
Ca2+ 0.43 ±0.25 1.25 ±0.76 0.32 ±0.08
NH4+ 6.49 ±3.78 5.99 ±2.20 1.05 ±0.32
SO42- 14.53 ±7.34 15.82 ±8.06 0.93 ±0.12
NO3- 9.04 ±5.49 8.83 ±5.02 1.01 ±0.17
Cl- 3.03 ±1.29 3.55 ±1.25 0.88 ±0.25
Acetate 2.33 ±2.38 4.40 ±4.60 0.66 ±0.35
Formate 0.01 ±0.01 0.19 ±0.08 n/a
Oxalate 0.29 ±0.11 0.30 ±0.13 1.04 ±0.31
± 1-sigma
Major ions represented
mainly in fine
fraction; bulk of
sodium and calcium in
coarse fraction
9
SheShan November 99Correlations with Wind, Wind Roses
N
E
S
W7.5 15
ppbv
NOy N
E
S
W10 20
ppbv
SO2
N
E
S
W3 6 m/s
Wind Speed
N
E
S
W3.5 7
%
WindFrequency
NOy indicative of influence from mobile sources, i.e.the Shanghai-Hangzhou Expressway to S and E,
and metropolitan Shanghai to NE
SO2 points to possible point sources to W and NE
10
SheShan November 99Meteorological, Trace Gas, and [PM2.5] Time Series
80
60
40
20
0
NO
NO
y O
3 (
pp
bv)
11/1/1999 11/6/1999 11/11/1999 11/16/1999 11/21/1999 11/26/1999 12/1/1999
Date (LT)
20
15
10
5
0
NO
3- (u
g/m3)
70
60
50
40
30
20
10
0
SO
4= (
ug/
m3 )
S
O2
(pp
bv) 350
300
250
200
150
100
50
0
Win
d D
irection (d
egN)
25
20
15
10
Tem
per
atu
re
(C
)
15
10
5
0
Win
d S
peed
(m/s)
11
SheShan PM2.5 and Met. Data November 99PCM Data
0
20
40
60
80
100
120
140
160
11
/2
11
/3
11
/4
11
/5
11
/6
11
/7
11
/8
11
/9
11
/10
11
/11
11
/12
11
/13
11
/14
11
/15
11
/16
11
/17
11
/18
11
/19
11
/20
11
/21
11
/22
11
/23
11
/24
11
/25
11
/26
11
/27
11
/28
11
/29
11
/30
Av
g
PM
2.5 [
ug
m-3]
0
10
20
30
40
50
60
70
80
O3 [p
pb
v]
Ca++ Na+ K+ NH4+ Cl-
NO3- SO4= Acetate Formate Oxalate
OC OOE EC O3-hrly max
0
5
10
15
20
25
11
/2
11
/3
11
/4
11
/5
11
/6
11
/7
11
/8
11
/9
11
/10
11
/11
11
/12
11
/13
11
/14
11
/15
11
/16
11
/17
11
/18
11
/19
11
/20
11
/21
11
/22
11
/23
11
/24
11
/25
11
/26
11
/27
11
/28
11
/29
11
/30
Av
g
T [o
C],
WS
[m
s-1
]
0
50
100
150
200
250
300
350
400
WD
[deg
]
Temperature Wind Speed Wind Direction
• Change in synoptic
conditions on 11/14 and 11/23
(cold fronts)accompanied by sharp drops in PM2.5 and O3, subsequent
recovery
• High mass on 11/24 due to agricultural
burning in close vicinity to the site
12
Sampling Locations in the Yangtze Delta
13
Regional Comparison of PM2.5 Composition
ChangShu Partisol November 99
0
20
40
60
80
100
120
140
160
11
/2
11
/3
11
/4
11
/5
11
/6
11
/7
11
/8
11
/9
11
/10
11
/11
11
/12
11
/13
11
/14
11
/15
11
/16
11
/17
11
/18
11
/19
11
/20
11
/21
11
/22
11
/23
11
/24
11
/25
11
/26
11
/27
11
/28
11
/29
11
/30
Av
g
PM
2.5 [
ug
m-3]
LinAn Andersen November 99
0
20
40
60
80
100
120
140
160
11/2
11/3
11/4
11/5
11/6
11/7
11/8
11/9
11/1
0
11/1
1
11/1
2
11/1
3
11/1
4
11/1
5
11/1
6
11/1
7
11/1
8
11/1
9
11/2
0
11/2
1
11/2
2
11/2
3
11/2
4
11/2
5
11/2
6
11/2
7
11/2
8
11/2
9
11/3
0
Av
g
PM
2.5
[u
g m
-3]
Ca++ Na+ K+ NH4+ Cl- NO3- SO4=
Acetate Formate Oxalate OC OOE EC
• Lowest levels at LinAn background
station,but temporal
fluctuations similar to ChangShu
• Regional influence by cold front
passages (11/14 and 11/23) noticeable at
both sites
• Signatures of sporadic local
influences on top of regional trend
14
Average Mass CompositionSheShan PCM November 99
NO3-11%
NH4+8%EC
3%
SO4=17%
Cl-4%
Organic Acids2%
OC36%
OOE15%
Na+0%
K+3%
Ca++1%
Average sum of components = 85.2 ug m-3
LinAn Andersen November 99
SO4=21%
NO3-8%
NH4+10%EC
4%
OC37%
OOE15%
Organic Acids1%
Na+0%
K+3%
Cl-1%
Ca++0%
Average sum of components = 75.7 ug m-3
ChangShu Partisol November 99
SO4=17%
NO3-9%
NH4+8%EC
3%
OC37%
OOE14%
Na+1%
K+3%
Ca++0%
Organic Acids
4% Cl-4%
Average sum of components = 112.3 ug m-3
No significant regional differences in November 99,
but noticeable seasonal differences at
ChangShu
ChangShu Partisol Spring 00
NO3-12%NH4+
11%
EC6%
SO4=25%
Cl-4%
Organic Acids
0%
Ca++0%
K+4%
Na+1%
OOE11%
OC26%
Average sum of components = 61.6 ug m-3
15
Seasonal/Regional Averages
PM2.5Charge Balance
-600
-400
-200
0
200
400
600
SheShan PCM Nov 99
LinAn Andersen Nov 99
ChangShu Partisol Nov 99
ChangShu Partisol Spring 00
[ne
m-3
]
SO4= NO3- NH4+ Net Acidity
• Seasonal differences in K+ due to post-harvest
biomass burning activities in November
• ChangShu highest Na+, Cl-, suggesting maritime influence
PM2.5 Concentrations
0102030405060708090
100110120
SheShan PCM Nov 99
LinAn Andersen Nov 99
ChangShu Partisol Nov 99
ChangShu Partisol Spring 00
Sta
cked
Co
nce
ntr
ati
on
s [u
g m
-3]
0
1
2
3
4
5
6
7
8
Ca
2+, N
a+, K
+, Cl - [u
g m
-3]
NH4+ NO3- SO4= Acetate Formate Oxalate OC
OOE EC Ca++ Na+ K+ Cl-
• Aerosol slightly acidic regionally; but lower variability at
LinAn
16
Comparison with Seasonal/Regional Averages at U.S. Sites
PM2.5 Mass Balance
0
5
10
15
20
25
30
35
40
AT
L P
M2.
5
AT
L O
3
HV
PM
2.5
HV
O3
DX
PM
2.5
DX
O3
HV
PM
2.5
HV
O3
DX
PM
2.5
DX
O3
HV
PM
2.5
HV
O3
DX
PM
2.5
DX
O3
[ug
m-3
]
0
20
40
60
80
100
120
[pp
bv]
Ca++ Na+ NH4+ Cl- NO3- SO4= AcetForm Oxal OC OOE EC Unid. O3-h max
Sum m er '99 Fall '99 Winter '99/'00
PM2.5 Charge Balance
-300
-200
-100
0
100
200
300
AT
L P
M 2
.5
HV
PM
2.5
DX
PM
2.5
HV
PM
2.5
DX
PM
2.5
HV
PM
2.5
DX
PM
2.5
[ne
m-3
]
SO4= NO3- NH4+ Net Acidity
Summer '99 Fall '99 Winter '99/'00
ATL: Atlanta, GA – urbanHV: H’ville, TN – suburbanDX: Dickson, TN - rural
• Significantly lower [PM2.5] at U.S. sites, even during
summer
• [O3] comparablein fall, much higher
in summer, esp.in urban Atlanta
•Slightly alkaline aerosolin fall and winter,
as opposed to Yangtze sites,probably due to different
emission patterns
17
Summary
• NH4+, SO4
2-, NO3-, and oxalate predominantly in fine mode (PM2.5); alkaline, alkaline earth
cations, Cl- and acetate represented indifferently between fine and coarse (PM10) modes
• Despite low photochemical activity during November period, O3 buildup along with PM2.5
concentrations after frontal passage
• During this buildup period, close correlation of gas phase SO2 and particle phase SO42- observed
• Apparent influence from roadways and point sources at SheShan indicated by NOy and SO2
• Average PM2.5 mass concentration levels highest at ChangShu, possibly due to close vicinity of
traffic sources; lowest in LinAn (background site)
• No regional differences in fine particle composition, but noticeable seasonal differences,
especially with respect to carbonaceous species and sulfate
• Seasonal differences most noticeable in K+ indicating influence of post-harvest burning in
November
• Significantly (~3x) lower PM2.5 in SE-US with tendency to slightly alcalinic aerosol in fall and
winter compared to slightly acidic conditions in the Yangtze Delta region
18
Acknowledgements
• Prof. Du HuiFang, Fudan University, ShangHai, for invaluable help preparing and
organizing the November intensive at SheShan
• Ms. Wu LiBo, Fudan University, ShangHai, for indispensable help and support at
the SheShan site
• Prof. Ding Guoan, CAMS Beijing, for patient help clearing research equipment
with Chinese customs
• The various local site operators at ChangShu, LinAn and SheShan for their
diligence and willingness to help us out with anything, anytime!!
19
SheShan November 99Diurnal Trends Related to Air Mass Transport
0.01
0.1
1
10
100
NO
(p
pb
v)
NO
0.8
0.6
0.4
0.2
0.0
NO
/NO
y (
-)
00:00 06:00 12:00 18:00
Time (LT)
NO/NOy
1
2
4
6
810
2
4
6
8100
NO
y (
pp
bv)
NOy
80
60
40
20
0
O3
(p
pb
v)
00:00 06:00 12:00 18:00
Time (LT)
O3
10
8
6
4
2
0Win
d Sp
eed
(m
/s)
10
8
6
4
2
0Win
d S
pee
d
(m/s
)
30025020015010050Wind Direction (deg)
Symbol code:
Size=WS / color=WD
• Winds driven by synoptic forces rather than convective
(no diurnal trend)
• Strong winds carry background [O3] ~30-40 ppbv
•NO peaks in morning and high levels carried into evening
• Weak photochemistry indicated by O3 and NO/NOy
20
PCM/Andersen Comparison SheShan 11/99 - Teflon
y = 0.6393x + 3.4553
R2 = 0.4913
0
2
4
6
8
10
12
14
16
18
0 2 4 6 8 10 12 14 16 18
PCM [ug m-3
]
Ande
rsen
[ug
m-3
]
NH4+ y = 1.3819x - 4.2158
R2 = 0.9064
0
5
10
15
20
25
30
35
0 5 10 15 20 25 30 35
PCM [ug m-3]
And
erse
n [u
g m
-3]
SO42-
y = 1.0185x - 0.5938
R2 = 0.839
0
5
10
15
20
25
0 5 10 15 20 25
PCM [ug m-3]
And
erse
n [u
g m
-3]
NO3-
21
PCM/Andersen Comparison SheShan 11/99 – Quartz
y = 0.9397x + 1.5508
R2 = 0.8943
0
10
20
30
40
50
60
70
80
0 10 20 30 40 50 60 70 80
PCM [ug m-3
]
And
erse
n [u
g m
-3]
OC y = 0.5211x + 0.7795
R2 = 0.6795
0
1
2
3
4
5
6
0 1 2 3 4 5 6
PCM [ug m-3]A
nder
sen
[ug
m-3
]
EC