SINCIERE Member Forum
Beijing, 2007.10.27-29
Emission and dispersion
of Polycyclic aromatic
hydrocarbons in China
S. Tao, Y.X. Zhang, C. Lang
Laboratory for Earth Surface Processes
Peking University
1. INTRODUCTION
2. EMISSION INVENTORY
3. DISPERSION MODELING IN GUANGDONG
PAH EMISSION IN CHINA
PAH CONTAMINATION IN CHINA
extensive contamination of various media
including food Mai et al., 2002; Shi et al., 2005; Wu et al., 2005;
Zhang et al., 2005; Zhu et al., 2005
particularly important in China both regionally
and globally Regionally Based Assessment of Toxic Substances,
UNEP Chemicals, 2003
LOCAL EXPOSURE RISK
1.00
3
1.0
- 0.3
0.75
Area
National Standard
Cumulative frequency
1.8 lg(ng/m )
0.50
0.25
0
0
9
Population
18
27
36
3
BaPeq, ng/m
National Standard 10 ng BaPeq/m3
Exceedence: 4% area, 41% population
BaPeq
China
Ambient air, 2m height, Tianjin
Tao et al., ES&T, 2006
LONG-RANGE TRANSPORT
Primbs et al., ES&T, 2007
OBJECTIVE
to develop an PAH emission inventory for China
to model the dispersion of PAHs in Guangdong
1. INTRODUCTION
2. EMISSION INVENTORY
3. DISPERSION MODELING IN GUANGDONG
METHODOLOGY
Emissions of individual PAHs and PAH16
NAP ACY ACE FLO PHE ANT FLA PYR BaA CHR BbF BkF BaP IcdP DahA BghiP
Fuel consumption at provincial level
Firewood, straw, domestic coal, industrial coal, coking, vehicle gas, other gas, natural gas
Modeling the fuel consumption
Prediction of fuel consumption at km2 resolution
Emission factors from the literature
Uncertainty analysis – Monte Carlo simulation
EMISSION DENSITY / INTENSICY
Emission density
Emission intensity
MAJOR EMISSION SOURCES
Small scale coke
27.2%
Large scale coke
production, 1.1%
Domestic coal, 6.8%
Industrial coal, 1.5%
Firewood
burning
Traffic oil, 2.5%
Al production, 0.9%
Consumer products, 0.9%
Others, 0.9%
21.2%
Indoor straw burning
Open fire
Straw burning
2.4%
34.6%
ENERGY CONSUMPTION MODELING
Ind coal
1.4E+05
7.0E+04
3.0E+04
Taiwan
Guangdong
0.0E+00
12500
GDP23
Industrial coal
25000
1.5E+04
Ind oil
0
Taiwan
7.0E+04
0
14000
GDP23
Industrial oil
2
= 0.7867
28000
3.5E+04
Henan 1.2E+04
0
Agri. Population,
Heilongjiang
15000
4000
Biofule
10000
8000
6.0E+03
Hebei
0.0E+00
5000
0
Guizhou
0
104
Traffic oil
0.0E+00
20000
Measured
R
BIofuel, 104 ton
0.0E+00
Sichuan
y = 6.844x
Hong Kong
0
10000
Observed
20000
Domestic coal
Based on population and temperature
Traffic oil
15000
GDP23
30000
MODEL VALIDATION
1.E+05
1.E+04
1.E+00
1.E+00
1.E+05
1.E+02
Model validation
1.E+05
1.E+00
1.E+00
1.E+02
1.E+04
Model validation
1.E+00
1.E+00
Model validation
1.E+05
MODEL UNCERTAINTY
40%
Relative Variation Index
Total Uncertainty
30%
Emission Activity Strength
20%
Emission Factors
10%
0%
OSC OSR OSW
Open-fire
straw burning
ISC
ISR
ISW
Indoor
straw burning
FWB DCA DCN
Firewood & coal
burning
LCP
SSP
Coke over
Relative variation index (RVI=SR(semi-interquartile ranges)/ median)
Range from 13.9% indoor straw burning to 37.6% small-scale coke production
Primarily from activity (straw) or emission factor (others)
EMISSION DENSITY km
2 resolution
Annual aerosol optical depth, MODIS
TEMPERAL CHANGE
140
Gasoline distribution
Open straws burning
Petroleum refinery
Al electrolysis
Industrial oil
Traffic oil
Industrial coal
Small-scale coke production
Large-scale coke production
Domestic coal
In-door straw
Firewood
2005
2000
1995
1990
1985
1980
1975
2005
2000
1995
1990
1985
1980
1975
1970
0
1965
0
1960
20
1955
5
1970
40
1965
10
60
1960
15
80
1955
20
100
1950
25
3
30
Firewood
In-door straw
Domestic coal
Small-scale coke production
Others
120
PAH16 Emission x 10 tons
35
1950
8
Emission activity strength x 10 tons
40
GLOBAL EMISSION preliminary
Continent/country
Emission
Percentage
Total World
521668
100.0%
Total Asia
289197
55.4%
151335
29.0%
89781
17.2%
125791
24.1%
114477
21.9%
46604
8.9%
97990
18.8%
Total Western and Central Africa
46604
8.9%
Total Eastern and Southern Africa
30235
5.8%
Total Northern Africa
21152
4.1%
46978
9.0%
41930
8.0%
32089
6.2%
2630
0.5%
Total Europe
49458
9.5%
Total South America
31398
6.0%
7664
1.5%
Total South and South-east Asia
India
Total East Asia
China
Total Western and Central Asia
Total Africa
Total North and Central America
Total North America
United States
Total Central America
Total Oceania
VALIDATION
1.E+04
1.E+04
1.E+05
transportation
1.E+04
1.E+03
1.E+03
1.E+03
Incineration
1.E+02
Incineration
1.E+02
1.E+02
1.E+01
Aluminum
Coking
1.E+01
1.E+01
1.E+00
Aviation ind.
Ind. coal
1.E+00
1.E+00 1.E+01 1.E+02 1.E+03 1.E+04 1.E+05
1.E+00
1.E+00
USA, 1990
UK, 1995
1.E-01
1.E+01
1.E+02
1.E+03
1.E+04
1.E-01
1.E+00
1.E+01
1.E+02
1.E+03
1.E+04
EU countries- BaP
GLOBAL EMISSION DENSITY preliminary
6
2.5
Residual, log(Gg/y)
Emission density, log(Gg/y)
EMISSION vs. GDP and Income
3
0
y = 0.85203 x - 3.60540
-3
y = -0.82529 x + 2.80241
0.5
-1.5
2
5
8
GDP, log(USD)
11
2
3
4
5
Income, log(USD/y)
LgEmission = 1.016 lgGDP – 0.961 lgIncome – 4.582
r2 = 0.843, n = 168,
SUMMARY
Total emission of PAH16 in China: 116,000 ton in 2003
10% carcinogenic compounds
Major sources: indoor biomass burning, small-scale coke ovens
Increased over time
Global emission of PAH16: 522,000 ton in 2003
1. INTRODUCTION
2. EMISSION INVENTORY
3. DISPERSION MODELING IN GUANGDONG
METHODOLOGY
Spatial resolved emission
Forward trajectories (HYSPLIT)
Partitioning, degradation, dry/wet deposition
Potential Receptor Influence Function (PRIF)
The probability of PAHs arriving at a receptor site, or cell, during
a given emission duration and a known period of transport time
EMISSION OF PHE, FLA, PYR, BaP in 2001
PHE
FLA
PYR
BaP
10.10
5.10
2.23
0.37
0
0
0
0
210,000 km2, over 80 million population
60 x 60 km2 resolution
China
Guangdong
50N
40N
50N
8km
10-12
10-6
100
4km
100E
110E
10-10
10-9
10-8
10-7
120E
10-6
130E
10-5
A 0-3day PRIF
140E
10-4
10-3
160E
10-2
100
0
0km
0km
150E
10-6
10S
0
10S
0
10S
90E
10-12
4km
4km
0km
80E
8km
10N
100
20N
30N
40N
30N
10-6
10N
10-12
10N
8km
20N
20N
30N
40N
50N
ANNUAL MEAN OUTFLOW OF PYRENE 2001
80E
90E
100E
110E
10-10
10-9
10-8
10-7
B
120E
10-6
130E
140E
10-5
3-5day PRIF
10-4
150E
10-3
160E
10-2
80E
90E
100E
110E
10-10
10-9
10-8
10-7
C
120E
10-6
130E
140E
10-5
10-4
150E
160E
10-3
5-7day PRIF
Annual mean PRIF (PYR) from Guangdong based on daily trajectory calculation
Total PRIF: 5.37x10-1, 2.56x10-3 and 8.92x10-5
10-2
50N
40N
Latitude
30N
6
0
2
4
Altitude (km)
8
10
0
10N
20N
30N
6
4
0
2
Altitude (km)
8
10
0
10N
20N
Latitude
40N
50N
SEASONAL VARIATION IN OUTFLOW
80E
10-10
90E
10-9
100E
110E
10-8
10-7
120E 130E
Longitude
F
10-6
10-5
140E
10-4
150E
10-3
160E
10-2
80E
10-10
90E
10-9
PRIF
Summer vs. winter
The East Asian monsoons domination
100E
110E
10-8
10-7
120E 130E
Longitude
10-6
E
10-5
PRIF
140E
10-4
150E
10-3
160E
10-2
90E
10-7
100E
10-6
110E
10-5
B
120E 130E
Longitude
10-4
PRIF
10-3
140E
10-2
150E
10-1
160E
50N
40N
0
10N
20N
29°N, 129°E
6
0
2
4
Altitude (km)
8
10
0
10
8
6
4
Altitude (km)
2
0
80E
30N
Latitude
40N
20N
10N
10N
0
10
8
6
4
2
0
Altitude (km)
30N
Latitude
30N
20N
Latitude
40N
50N
50N
SPECIAL WEATHER CONDITIONS
80E
90E
-10
-9
10
10
100E
-8
10
110E
-7
10
B
120E 130E
Longitude
-6
10
PRIF
-5
10
140E
150E
-4
10
10
160E
-3
-2
10
80E
90E
-10
-9
10
10
100E
-8
10
110E
120E 130E
Longitude
-7
10
B
-6
10
-5
10
140E
150E
-4
10
10
160E
-3
PRIF
Stagnation (May 7, 2001), typhoon (July 6, 2001), uplifting (Jan. 23, 2001)
One day emission, 5 days transport
10-2
INTERANNUAL VARIATION PYRENE
50N
2.4×10-2 P1
1.2×10-2
40N
0
P3
P2
30N
1.2×10
-4
P1
0
20N
P3
2.5×10-5
10N
P2
0
2 ONI
0
0
B
0-5 day transport period, three sites representing source and receptor regions
PRIFs peaked in Dec. in southeast Asia (P2) and in July in northern China (P3)
Abnormally high (low) PRIF – cold (warm) episodes (Ocean Nino Index)
04Jul
04Jan
03Jul
03Jan
02Jul
02Jan
01Jul
01Jan
00Jul
00Jan
99Jul
99Jan
98Jul
98Jan
97Jul
97Jan
96Jul
96Jan
95Jul
95Jan
94Jul
160E
94Jan
150E
93Jul
140E
93Jan
130E
92Jul
120E
A
92Jan
110E
91Jul
100E
91Jan
90E
90Jul
80E
90Jan
10S
-2
MODELING FOR CHINA, PRELIMINARY
Forward trajectory, PRIF
PRIF of PYR and BaP
2000
2000
1800
1600
1400
1200
1000
800
600
400
200
0
1800
1600
1400
1200
1000
800
600
400
200
0
85%
90%
95%
100%
85%
90%
95%
Euler atmospheric transport model
coupled with a fugacity multi-media model
Resolution: 24 km x 24km x 12 min
1.5, 3.9, 10, 100, 500, 1000, 2000, 3000, 7000 m
Annual mean conc. at 1.5 m height, log(pg/m3
100%
SUMMARY
48% remained in Guangdong under 200 m in 5 days
PAHs traveled to south and southeast predominantly
Strong seasonality
Occasionally uplifted and traveled toward the Pacific
ACKNOWLEDGEMENT
FINANCIAL SUPPORT
NATIONAL SCIENTIFIC FOUNDATION OF CHINA