Supplement of Insights into aerosol chemistry during the 2015 China

Supplement of Atmos. Chem. Phys., 17, 3215–3232, 2017
http://www.atmos-chem-phys.net/17/3215/2017/
doi:10.5194/acp-17-3215-2017-supplement
© Author(s) 2017. CC Attribution 3.0 License.
Supplement of
Insights into aerosol chemistry during the 2015 China Victory Day
parade: results from simultaneous measurements at ground level and 260 m
in Beijing
Jian Zhao et al.
Correspondence to: Yele Sun ([email protected])
The copyright of individual parts of the supplement might differ from the CC-BY 3.0 licence.
Table S1. Summary of the average meteorological parameters and mass concentrations of PM1 species during the five polluted episodes and
two clean periods (Fig. 6) at ground level and 260 m.
260 m
PE1
PE2
C1
PE3
Ground
PE4
PE5
C2
PE1
PE2
C1
PE3
PE4
PE5
C2
Meteorological Parameters
T (oC)
RH (%)
-1
WS (m s )
22.72
21.94
21.84 20.40
21.72
20.70
18.49
24.90
24.38
23.73
22.67
23.35
22.19
20.01
78.44
77.25
75.16 96.26
63.91
65.75
55.13
67.26
66.42
68.48
84.82
60.83
62.80
56.62
2.14
2.82
4.44
3.08
3.06
3.12
4.88
1.34
1.26
1.17
1.29
1.06
1.08
1.41
-3
Aerosol Species (μg m )
Org
11.84
11.73
4.58
12.11
20.40
22.69
3.97
12.77
13.17
9.27
16.61
24.93
32.35
7.81
POA
3.92
3.99
1.57
3.95
6.94
7.42
1.47
4.02
3.28
4.32
4.07
7.33
8.49
4.01
SOA
7.93
7.73
3.01
8.16
13.45
15.27
2.49
8.75
9.89
4.94
12.54
17.59
23.86
3.81
SO4
6.68
3.93
1.02
5.11
6.16
12.42
0.70
10.41
6.31
2.53
11.18
9.37
23.46
1.22
NO3
10.03
5.07
0.79
10.43
10.02
15.79
0.54
10.85
5.49
1.51
14.96
9.38
19.96
0.94
NH4
4.69
2.69
0.68
4.52
4.62
8.28
0.48
6.53
3.48
1.13
8.20
5.73
13.36
0.56
Chl
0.45
0.24
0.08
0.69
0.44
0.72
0.07
0.28
0.13
0.05
0.65
0.39
0.85
0.05
BC
2.39
1.56
0.67
2.43
4.01
6.24
0.66
1.66
1.51
0.94
1.98
3.75
4.51
1.01
PM1
36.09
25.21
7.82
35.29
45.63
66.13
6.41
42.50
30.08
15.43
53.57
53.55
94.49
11.58
2
(a)
315
(b)
0
0.4
0.3
45
0
0.25
315
0.15
0.2
0.1
0.1
0
270
225
180
45
0.2
0.05
0.1 0.2 0.3 0.4
0 2 135 4 6 8 10+
90
270
2
4
6
8
10
0
0.05 0.1 0.15 0.2 0.25
225
90
135
180
Figure S1.Wind rose plots (a) during the control period (20 August – 3 September) and (b) after the
control period (4 September – 30 September), which are colored by wind speed (m s-1).
25
(a)
(b)
2
r =0.99
15
20
10
-3
10
-3
15
5
AE 22 (µg m )
-3
10
AE 22 (µg m )
AE 33 (µg m )
line 1:1
Slope=0.72
12
8
6
4
5
2
0
5
0
0:00 6:00 12:00 18:00 0:00 6:00 12:00 18:00 0:00 6:00 12:00 18:00
10/14
10/15
10/13
Date & Time
0
0
5
10
-3
15
AE 33 (µg m )
Figure S2. (a) Time series and (b) Scatter plot of BC derived from AE 22 and AE33 at 880 nm.
3
(a)
40
(b)
Slope=0.88
20
line 1:1
2
2
-3
30
20
2015-9-30
2015-9-20
2015-9-10
2015-8-31
10
0
15
10
2015-9-30
2015-9-20
2015-9-10
2015-8-31
5
Date & Time
NH4 Measured (µg m )
-3
r =0.98
Date & Time
NH4 Measured (µg m )
line 1:1
Slope=0.85
r =1.00
0
0
10
20
30
-3
NH4 Predicted (µg m )
0
40
5
10
15
20
-3
NH4 Predicted (µg m )
25
Figure S3. Scatter plots of measured ammonium versus the predicted ammonium that requires to fully
neutralize sulfate, nitrate and chloride at (a) ground level and (b) 260 m.
Elemental Ratios, I-A method
3.0
2.5
H/C
2
r = 0.958
Slope = 1.09
2.0
OM/OC
O/C
1.5
2
2
r = 0.993
Slope = 1.10
r = 0.993
Slope = 1.27
1.0
0.5
0.0
0.0
0.5
1.0
1.5
2.0
2.5
Elemental Ratios, A-A method
5
Figure S4. Scattering plot of elemental ratios, including oxygen-to-carbon (O/C), hydrogen-to-carbon
(H/C) and organic mass–to–organic carbon (OM/OC) ratio calculated from the I-A method
(Canagaratna et al., 2015) versus those from the A-A method (Aiken et al., 2007;Aiken et al., 2008).
4
(b) 0.0
(a)
0.7
Mass Fraction
Q/Qexpected
0.8
0.6
0.5
0.4
0.3
Scaled Residual
1
2
2
3
4
5
6
Number of Factors
8
0.4
OOA
0.6
0.8
1.0
-1 -0.8-0.6-0.4-0.2 0 0.2 0.4 0.6 0.8 1
fPeak
(c)
0
-2
20
-3
Mass Conc. (µg m )
7
HOA
0.2
40
30
40
50
(d)
60
70
m/z (amu)
80
90
100
110
120
30
20
10
0
2015-8-26
2015-9-15
Date & Time
2015-9-25
Σ abs(Resid)/ΣTotal
Σ Abs(Resid)
2 2
Σ (Resid /σ )/Qexp
Σ Resid/ΣTotal
Σ Resid
4
2
0
-2
2015-9-5
(e)
10
8
6
4
2
0
4
2
0
-2
-4
8
6
4
2
0
6
4
2
0
2015-8-26
2015-9-5
2015-9-15
2015-9-25
Date & Time
5
Figure S5. Summary of the main diagnostic plots of the two-factor PMF resolution of ACSM organic
matrix at 260 m: (a) Q/Qexpected varied as a function of the number of factors, (b) mass fraction of the
two OA factors (i.e. HOA and OOA) as a function of fPeak, (c) box plot of scaled residual for each m/z,
(d) time series of measured mass comcentrations comparing with the reconstructed ones by the twofactor PMF solution at fPeak=0, (e) time series of the resisual diagnostics.
5
(b)
Mass Fraction
15
10
5
1
(d)
2
3 4 5 6 7 8
Number of Factors
9 10
0.2
0.4
COA
LO-OOA
0.6
0.8
1.0
MO-OOA
200
(f)
Scaled Residual
150
100
50
0
-50
-100
-150
(e)
-3
Mass Conc. (µg m )
80
20
40
60
80
m/z (amu)
100
120
Measured Signal
Reconst Signal
60
HOA
0.2
0.4
0.6
0.8
OOA
-1 -0.8-0.6-0.4-0.2 0 0.2 0.4 0.6 0.8 1
fPeak
2
1
0
-1
5
4
3
2
1
0
0.2
0.1
0.0
-0.1
0.30
0.20
0.10
40
0.00
120
80
40
0
20
0
2015-8-26
2015-9-5
2015-9-15
Date & Time
2015-9-25
2015-9-5
2015-9-15
Date & Time
2015-8-26
2015-9-25
Figure S6. Summary of the main diagnostic plots of the four-factor PMF resolution of HR-AMS
organic matrix at ground: (a) Q/Qexpected varied as a function of the number of factors, (b) mass fraction
of four OA factors as a function of fPeak, (c) mass fraction of two OA facors as a function of fPeak, (d)
box plot of scaled residual for each fragment ion, (e) time series of measured mass comcentrations
comparing with that reconstructed by the four-factor PMF solution at fPeak=0, (f) time series of the
resisual diagnostics.
+
% of Total Signal
5
0.0
1.0
-1 -0.8-0.6-0.4-0.2 0 0.2 0.4 0.6 0.8 1
fPeak
Σ abs(Resid)/ΣTotal
Σ Abs(Resid)
2 2
Σ (Resid /σ )/Qexp
Σ Resid/ΣTotal
Q/Qexpected
20
(c)
HOA
Mass Fraction
0.0
Σ Resid
(a)
+
+
+
+
CxHy CxHyO1 CxHyO2 HyO1 CxHyNp CxHyOzNp
10
8
6
4
2
0
+
HOA
(a)
O/C = 0.14
H/C = 1.85
N/C = 0.002
OM/OC = 1.35
OOA
(b)
15
O/C = 1.16
H/C = 1.65
N/C = 0.012
OM/OC = 2.67
10
5
0
10
20
30
40
50
60
m/z (amu)
70
80
90
100
Figure S7. High resolution mass spectra of OA factors from two-factor PMF solution at ground level.
6
0.8
(a)
0.4
HOA
2
0.2
NO3 SO4 NH4
Chl
BC
NO2 NOx
O3
RH
0.0
Ox
0.8
(c)
LO-OOA
2
0.4
R
2
NO3 SO4 NH4
Chl
BC
NO2 NOx
O3
RH
(d)
Ox
MO-OOA
0.6
0.6
R
0.2
0.1
0.0
0.8
COA
0.3
0.4
R
R
2
0.6
(b)
0.4
0.2
0.2
0.0
NO3 SO4 NH4
Chl
BC
NO2 NOx
O3
RH
0.0
Ox
NO3 SO4 NH4
Chl
BC
NO2 NOx
O3
RH
Ox
-3
-3
SMPS (15-400 nm)
ACSM+AE33
(b)
100
50
2
SMPS (15-600 nm)
ACSM+AE33
S=0.91; R =0.92
80
(c)
100
50
40
-1
0
800
600
400
200
0
2
CAPS
ACSM+AE33
R =0.76
(d)
0
150
100
50
-3
PM1 (µg m )
Ext. (M m )
0
150
-3
SMPS (µg m )
2
S=0.69; R =0.94
100
80
60
40
20
0
150
PM1 (µg m )
80
60
40
20
0
120
(a)
-3
1.6
1.5
1.4
1.3
1.2
PM1 (µg m )
Density (g cm )
Figure S8. Correlations of the four OA factors of HR-AMS: (a) HOA, (b) COA, (c) LO-OOA and (d)
MO-OOA with external tracers during the entire study.
0
8/22
8/26
8/30
9/3
9/7
9/11
9/15
9/19
9/23
9/27
10/1
Date & Time
5
Figure S9. (a) Time series of particle density, and inter-comparisons between PM1 (= NR-PM1 + BC)
and (b) mass concentrations converted from 15-400 nm and (c) from 15-600 nm particles that derived
from SMPS measurements, and (d) light extinction coefficient of PM2.5. The correlation coefficients (R2)
and regression slopes (S) are also given in (b-d).
7
(a)
(b)
80
Slope=0.45
Slope=0.91
2
R =0.94
2015-9-30
2015-9-20
2015-9-10
2015-8-31
20
10
Date & Time
30
-3
-3
40
60
40
2015-9-30
2015-9-20
2015-9-10
2015-8-31
20
0
Date & Time
SMPS15-400nm (µg m )
-3
50
50
100
150
-3
PM1 (µg m )
R =0.92
80
60
40
20
0
0
line 1:1
2
100
R =0.94
60
SMPS15-400nm (µg m )
(c)
line 1:1
Slope=0.69
2
SMPS15-600nm (µg m )
70
0
0
200
20
40
60
80
-3
PM1 (µg m )
100
0
120
20
40
60
80
-3
PM1 (µg m )
100
120
Figure S10. Scatter plots of PM1 measured by HR-AMS/ACSM and AE versus the mass concentrations
converted from the number concentrations of SMPS measurements in different size ranges: (a) 15-400
nm at ground level, (b) 15-400 nm at 260 m, and (c) 15-600 nm at 260 m.
50
Slope=0.64
(a)
(b)
2
r =0.62
Slope=0.47
(c) 40
2
r =0.80
Slope=0.61
2
r =0.71
-3
NO3, 260 m (µg m )
-3
SO4, 260 m (µg m )
20
-3
Org, 260 m (µg m )
40
25
30
20
2015-9-30
2015-9-10
Date
2015-9-20
10
15
10
30
20
10
5
2015-8-31
0
0
20
(e)
2
r =0.76
15
0
0
80
4
10
20
30
-3
SO4, Ground (µg m )
Slope=0.65
0
40
16
(f) 14
2
r =0.59
3
10
5
10
20
30
40
50
-3
NO3, Ground (µg m )
Slope=1.01
60
70
2
r =0.77
12
-3
-3
Chl, 260 m (µg m )
-3
NH4, 260 m (µg m )
(d)
20
40
60
-3
Org, Ground (µg m )
Slope=0.52
BC, 260 m (µg m )
0
2
1
10
8
6
4
2
0
0
0
5
5
10
15
20
25
-3
NH4, Ground (µg m )
30
35
0
0
2
4
6
-3
Chl, Ground (µg m )
8
0
2
4
6
8
-3
10
12
BC, Ground (µg m )
Figure S11. Scatter plots of PM1 species measured at 260 m versus those measured at ground.
8
1.0
0.7
(a)
0.8
1.0
0.5
0.6
0.4
0.8
0.4
0.3
0.2
0.6
0.2
2.0
0
4
8
12
16
20
0.2
SO4
0.0
24
0
1.0
(d)
1.5
(c)
0.4
0.1
Org
0.0
R260m/Ground
1.2
(b)
0.6
4
8
12
16
20
(e)
0.8
NO3
0.0
24
0
4
8
12
16
20
24
(f)
0.6
1.0
0.4
0.5
0.2
POA
0.0
NH4
0.0
0
4
(g)
8
12
16
20
24
0
4
8
12
16
20
24
(h)
1.2
(i)
1.0
0.8
0.6
0.4
0.2
BC
0.0
0
4
8
12
16
20
24
Hour of Day
Figure S12. Diurnal variations of the ratios of 260 m to ground (R260m/Ground) for each species.
References
5
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