Emission Emission andand dispersion of dispersion of
Polycyclic aromatic Polycyclic aromatic hydrocarbons in Chinahydrocarbons in China
S. Tao, Y.X. Zhang, C. LangS. Tao, Y.X. Zhang, C. LangLaboratory for Earth Surface ProcessesLaboratory for Earth Surface Processes
Peking UniversityPeking University
SINCIERE Member ForumBeijing, 2007.10.27-29
11111. INTRODUCTION
2. EMISSION INVENTORY
3. DISPERSION MODELING IN GUANGDONG
1. INTRODUCTION
2. EMISSION INVENTORY
3. DISPERSION MODELING IN GUANGDONG
PAH EMISSION IN CHINAPAH EMISSION IN CHINA
PAH CONTAMINATION IN CHINAPAH CONTAMINATION IN CHINA
extensive contamination of various media extensive contamination of various media
including food including food Mai et al., 2002; Shi et al., 2005; Wu et al., 2005; Mai et al., 2002; Shi et al., 2005; Wu et al., 2005;
Zhang et al., 2005; Zhu et al., 2005Zhang et al., 2005; Zhu et al., 2005
particularly important in China both regionally particularly important in China both regionally
and globally and globally Regionally Based Assessment of Toxic Substances, Regionally Based Assessment of Toxic Substances,
UNEP Chemicals, 2003UNEP Chemicals, 2003
BaPeq
1.8 lg(ng/m 3 )
- 0.3
1.0
LOCAL EXPOSURE RISKLOCAL EXPOSURE RISK
ChinaChina
Ambient air, 2m height, TianjinAmbient air, 2m height, Tianjin
Area
1.00
Cu
mu
lati
ve
freq
uen
cy
0 0 36
BaPeq, ng/m3
0.75
0.25
18 9 27
0.50 Population
Nat
iona
l S
tand
ard
National Standard 10 ng BaPeq/mNational Standard 10 ng BaPeq/m33
Exceedence: 4% area, 41% populationExceedence: 4% area, 41% population
Tao et al., ES&T, 2006Tao et al., ES&T, 2006
LONG-RANGE TRANSPORTLONG-RANGE TRANSPORT
Primbs et al., ES&T, 2007Primbs et al., ES&T, 2007
OBJECTIVEOBJECTIVE
to develop an PAH emission inventory for Chinato develop an PAH emission inventory for China
to model the dispersion of PAHs in Guangdongto model the dispersion of PAHs in Guangdong
22221. INTRODUCTION
2. EMISSION INVENTORY
3. DISPERSION MODELING IN GUANGDONG
1. INTRODUCTION
2. EMISSION INVENTORY
3. DISPERSION MODELING IN GUANGDONG
METHODOLOGYMETHODOLOGY
Emission factors from the literatureEmission factors from the literature
Emissions of individual PAHs and PAHEmissions of individual PAHs and PAH1616
NAP ACY ACE FLO PHE ANT FLA PYR BaA CHR BbF BkF BaP IcdP DahA BghiP
Fuel consumption at provincial levelFuel consumption at provincial levelFirewood, straw, domestic coal, industrial coal, coking, vehicle gas, other gas, natural gas
Uncertainty analysis – Monte Carlo simulationUncertainty analysis – Monte Carlo simulation
Modeling the fuel consumptionModeling the fuel consumption
Prediction of fuel consumption at kmPrediction of fuel consumption at km22 resolution resolution
EMISSION DENSITY / INTENSICYEMISSION DENSITY / INTENSICY
Emission intensityEmission intensityEmission intensityEmission intensity
Emission densityEmission densityEmission densityEmission density
MAJOR EMISSION SOURCESMAJOR EMISSION SOURCES
Al production, 0.9%Consumer products, 0.9%
Others, 0.9%
Traffic oil, 2.5%
Large scale coke production, 1.1%
Domestic coal, 6.8%
Industrial coal, 1.5%
Small scale coke
27.2%
Firewood burning
21.2%
Open fire Straw burning
2.4%
Indoor straw burning
34.6%
0.0E+00
7.0E+04
1.4E+05
0 12500 25000GDP23
Ind
coal
Taiwan
0.0E+00
1.5E+04
3.0E+04
0 14000 28000GDP23
Ind
oil
Taiwan
Hong Kong
Guangdong
ENERGY CONSUMPTION ENERGY CONSUMPTION MODELINGMODELING
Domestic coalDomestic coalBased on population and temperatureBased on population and temperature
0
5000
10000
15000
20000
0 10000 20000
Heilongjiang
Hebei
Guizhou
Observed
Mea
sure
d
0.0E+00
3.5E+04
7.0E+04
0 4000 8000
Agri. Population, 104
BIo
fuel
, 104
ton
y = 6.844x
R2 = 0.7867
Henan
Sichuan
0.0E+00
6.0E+03
1.2E+04
15000 300000GDP23
Tra
ffic
oil
Industrial coalIndustrial coal
Industrial oilIndustrial oil
BiofuleBiofule
Traffic oilTraffic oil
MODEL VALIDATIONMODEL VALIDATION
1.E+00
1.E+05
1.E+00 1.E+05
1.E+00
1.E+02
1.E+04
1.E+00 1.E+02 1.E+04
1.E+00
1.E+05
1.E+00 1.E+05
Model validationModel validation
Model validationModel validation
Model validationModel validation
MODEL UNCERTAINTYMODEL UNCERTAINTY
Relative variation index (RVI=SRRelative variation index (RVI=SR(semi-interquartile ranges)(semi-interquartile ranges)/ median)/ median)
Range from 13.9% Range from 13.9% indoor straw burningindoor straw burning to to 37.6%37.6% small-scale coke production small-scale coke production
Primarily from activity (straw) or emission factor (others)Primarily from activity (straw) or emission factor (others)
0%
10%
20%
30%
40%
OSC OSR OSW ISC ISR ISW FWB DCA DCN LCP SSP
Rela
tive V
ariatio
n I
ndex
Total Uncertainty
Emission Activity Strength
Emission Factors
Open-fire straw burning
Indoor straw burning
Firewood & coal burning
Coke over
EMISSION DENSITY EMISSION DENSITY kmkm22 resolution resolution
Annual aerosol optical depth, MODISAnnual aerosol optical depth, MODIS
TEMPERAL CHANGETEMPERAL CHANGE
35
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
Em
issi
on a
ctiv
ity s
tren
gth
x 1
08 to
ns
2005
30
25
20
15
10
5
0
40
2000
1995
1990
1985
1980
1975
1970
1965
1960
1955
1950
Others Small-scale coke production Domestic coal In-door straw Firewood
PA
H1
6 E
mis
sion
x 1
03 tons
140
120
100
80
60
40
20
0
2005
2000
1995
1990
1985
1980
1975
1970
1965
1960
1955
1950
GLOBAL EMISSION GLOBAL EMISSION preliminarypreliminary
Continent/country Emission Percentage
Total World 521668 100.0%
Total Asia 289197 55.4%
Total South and South-east Asia 151335 29.0%
India 89781 17.2%
Total East Asia 125791 24.1%
China 114477 21.9%
Total Western and Central Asia 46604 8.9%
Total Africa 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%
Total North and Central America 46978 9.0%
Total North America 41930 8.0%
United States 32089 6.2%
Total Central America 2630 0.5%
Total Europe 49458 9.5%
Total South America 31398 6.0%
Total Oceania 7664 1.5%
VALIDATIONVALIDATION
1.E+00
1.E+01
1.E+02
1.E+03
1.E+04
1.E+05
1.E+00 1.E+01 1.E+02 1.E+03 1.E+04 1.E+05
USA, 1990 USA, 1990
1.E+00
1.E+01
1.E+02
1.E+03
1.E+04
1.E+00 1.E+01 1.E+02 1.E+03 1.E+04
UK, 1995UK, 1995
1. E- 01
1. E+00
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 EU countries- BaP
Incineration
transportation
Aviation ind.
Coking
Incineration
Ind. coal
Aluminum
GLOBAL EMISSION DENSITY GLOBAL EMISSION DENSITY preliminarypreliminary
EMISSION vs. GDP and IncomeEMISSION vs. GDP and Income
-3
0
3
6
2 5 8 11-1.5
0.5
2.5
2 3 4 5
Em
issi
on d
ensi
ty,
log(
Gg
/y)
Res
idua
l, lo
g(G
g/y)
GDP, log(USD) Income, log(USD/y)
y = -0.82529 x + 2.80241
y = 0.85203 x - 3.60540
LgEmission = 1.016 lgGDP – 0.961 lgIncome – 4.582 r2 = 0.843, n = 168,
SUMMARYSUMMARY
Total emission of PAHTotal emission of PAH1616 in China: 116,000 ton in 2003 in China: 116,000 ton in 2003
10% carcinogenic compounds10% carcinogenic compounds
Major sources: Major sources: indoor biomass burning, small-scale coke ovensindoor biomass burning, small-scale coke ovens
Increased over timeIncreased over time
Global emission of PAHGlobal emission of PAH1616: 522,000 ton in 2003: 522,000 ton in 2003
33331. INTRODUCTION
2. EMISSION INVENTORY
3. DISPERSION MODELING IN GUANGDONG
1. INTRODUCTION
2. EMISSION INVENTORY
3. DISPERSION MODELING IN GUANGDONG
METHODOLOGYMETHODOLOGY
Spatial resolved emissionSpatial resolved emission
Potential Receptor Influence Function (PRIF)Potential Receptor Influence Function (PRIF)
Forward trajectories (HYSPLIT)Forward trajectories (HYSPLIT)
Partitioning, degradation, dry/wet deposition Partitioning, degradation, dry/wet deposition
The probability of PAHs arriving at a receptor site, or cell, during The probability of PAHs arriving at a receptor site, or cell, during a given emission duration and a known period of transport timea given emission duration and a known period of transport time
EMISSION OF PHE, FLA, PYR, BaP iEMISSION OF PHE, FLA, PYR, BaP in 2001n 2001
PHE
0
10.10
FLA
0
5.10
PYR
0
2.23
BaP
0
0.37
210,000 km210,000 km22, over 80 million population, over 80 million population
60 x 60 km60 x 60 km22 resolution resolution
ChinaChina
GuangdongGuangdong
ANNUAL MEAN OUTFLOW OF ANNUAL MEAN OUTFLOW OF PYRENE PYRENE 20012001
10S
0 10
N
20N
30
N
40N
50
N
90E 100E 110E 120E 130E 140E 150E 160E 80E
10-10 10-9 10-8 10-7 10-6 10-5 10-4 10-3 10-2
A 0-3day PRIF
0km
4km
8km 10-12 10-6 100
10S
0 10
N
20N
30
N
40N
50
N
90E 100E 110E 120E 130E 140E 150E 160E 80E
10-10 10-9 10-8 10-7 10-6 10-5 10-4 10-3 10-2
0km
4km
8km 10-12 10-6 100
B 3-5day PRIF
10S
0 10
N
20N
30
N
40N
50
N
90E 100E 110E 120E 130E 140E 150E 160E 80E
10-10 10-9 10-8 10-7 10-6 10-5 10-4 10-3 10-2
0km
4km
8km 10- 12 10- 6 100
C 5-7day PRIF
Annual mean PRIF (PYR) from Guangdong based on daily trajectory calculationAnnual mean PRIF (PYR) from Guangdong based on daily trajectory calculation
Total PRIF: 5.37x10Total PRIF: 5.37x10-1-1, 2.56x10, 2.56x10-3-3 and 8.92x10 and 8.92x10-5-5
SEASONAL VARIATION IN SEASONAL VARIATION IN OUTFLOWOUTFLOW
0 10
N
20N
30
N
40N
50
N
90E 100E 110E 120E 130E 140E 150E 160E 80E
10-10 10-9 10-8 10-7 10-6 10-5 10-4 10-3 10-2
Alt
itud
e (k
m)
0 2
10
4 6
8
Lat
itud
e
Longitude
E PRIF
0 10
N
20N
30
N
40N
50
N
90E 100E 110E 120E 130E 140E 150E 160E 80E
10-10 10-9 10-8 10-7 10-6 10-5 10-4 10-3 10-2
Alt
itud
e (k
m)
0 2
10
4 6
8
Lat
itud
e
Longitude
F PRIF
Summer vs. winterSummer vs. winter
The East Asian monsoons dominationThe East Asian monsoons domination
SPECIAL WEATHER CONDITIONSSPECIAL WEATHER CONDITIONS
0 10
N
20N
30
N
40N
50
N
90E 100E 110E 120E 130E 140E 150E 160E 80E
10-10 10-9 10-8 10-7 10-6 10-5 10-4 10-3 10-2
Alti
tude
(km
)
0 2
10
4 6
8
Lat
itude
Longitude
B PRIF
29°N, 129°E
0 10
N
20N
30
N
40N
50
N
90E 100E 110E 120E 130E 140E 150E 160E 80E
10-7 10-6 10-5 10-4 10-3 10-2 10-1
Alt
itud
e (k
m)
0 2
10
4 6
8
Lat
itud
e
Longitude
B PRIF
0 10
N
20N
30
N
40N
50
N
90E 100E 110E 120E 130E 140E 150E 160E 80E
10-10 10-9 10-8 10-7 10-6 10-5 10-4 10-3 10-2
Alt
itud
e (k
m)
0 2
10
4 6
8
Lat
itud
e
Longitude
B PRIF
Stagnation (May 7, 2001), typhoon (July 6, 2001), uplifting (Jan. 23, 2001) Stagnation (May 7, 2001), typhoon (July 6, 2001), uplifting (Jan. 23, 2001)
One day emission, 5 days transportOne day emission, 5 days transport
INTERANNUAL VARIATION INTERANNUAL VARIATION PYRENEPYRENE
0-5 day transport period, three sites representing source and receptor regions0-5 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)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)Abnormally high (low) PRIF – cold (warm) episodes (Ocean Nino Index)
10S
0 10
N
20N
30
N
40N
50
N
90E 100E 110E 120E 130E 140E 150E 160E 80E
P1
P2
P3
A
90
Jan
90
Jul
91
Jan
91
Jul
92
Jan
92
Jul
93
Jan
93
Jul
94
Jan
94
Jul
95
Jan
95
Jul
96
Jan
96
Jul
97
Jan
97
Jul
98
Jan
98
Jul
99
Jan
99
Jul
00
Jan
00
Jul
01
Jan
01
Jul
02
Jan
02
Jul
03
Jan
03
Jul
04
Jan
04
Jul
2.4× 10-2
1.2× 10-2
0
1.2× 10-4
0
2.5× 10-5
0
0
-2
2
P1
P2
P3
ONI
B
MODELING FOR CHINA, MODELING FOR CHINA, PRELIMINARYPRELIMINARY
0
200
400
600
800
1000
1200
1400
1600
1800
2000
85% 90% 95% 100%
0
200
400600
800
1000
1200
14001600
1800
2000
85% 90% 95% 100%
Forward trajectory, PRIFForward trajectory, PRIF
PRIF of PYR and BaPPRIF of PYR and BaP
Resolution: 24 km x 24km x 12 minResolution: 24 km x 24km x 12 min
Euler atmospheric transport modelEuler atmospheric transport model
Annual mean conc. at 1.5 m height, log(pg/mAnnual mean conc. at 1.5 m height, log(pg/m33
coupled with a fugacity multi-media modelcoupled with a fugacity multi-media model
1.5, 3.9, 10, 100, 500, 1000, 2000, 3000, 7000 m1.5, 3.9, 10, 100, 500, 1000, 2000, 3000, 7000 m
SUMMARYSUMMARY
48% remained in Guangdong under 200 m in 5 days48% remained in Guangdong under 200 m in 5 days
PAHs traveled to south and southeast predominantlyPAHs traveled to south and southeast predominantly
Strong seasonalityStrong seasonality
Occasionally uplifted and traveled toward the PacificOccasionally uplifted and traveled toward the Pacific
FINANCIAL SUPPORTFINANCIAL SUPPORTNATIONAL SCIENTIFIC FOUNDATION OF CHINANATIONAL SCIENTIFIC FOUNDATION OF CHINA
ACKNOWLEDGEMENTACKNOWLEDGEMENT
