Emission and dispersion of Polycyclic aromatic hydrocarbons in China S. Tao, Y.X. Zhang, C. Lang Laboratory for Earth Surface Processes Peking University SINCIERE Member Forum Beijing,

11 1.INTRODUCTION 2.EMISSION INVENTORY 3.DISPERSION MODELING IN GUANGDONG 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

BaPeq 1.8 lg(ng/m 3 ) LOCAL EXPOSURE RISK China Ambient air, 2m height, Tianjin National Standard 10 ng BaPeq/m 3 Exceedence: 4% area, 41% population 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

22 1.INTRODUCTION 2.EMISSION INVENTORY 3.DISPERSION MODELING IN GUANGDONG 1.INTRODUCTION 2.EMISSION INVENTORY 3.DISPERSION MODELING IN GUANGDONG

METHODOLOGY Emission factors from the literature Emissions of individual PAHs and PAH 16 NAPACYACEFLOPHEANTFLAPYRBaACHRBbFBkFBaPIcdPDahABghiP Fuel consumption at provincial level Firewood, straw, domestic coal, industrial coal, coking, vehicle gas, other gas, natural gas Uncertainty analysis – Monte Carlo simulation Modeling the fuel consumption Prediction of fuel consumption at km 2 resolution

EMISSION DENSITY / INTENSICY Emission intensity Emission density

MAJOR 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 E E GDP23 Ind coal Taiwan 0.0E E E GDP23 Ind oil Taiwan Hong Kong Guangdong ENERGY CONSUMPTION MODELING Domestic coal Based on population and temperature Heilongjiang Hebei Guizhou Observed Measured 0.0E E E Agri. Population, 10 4 BIofuel, 10 4 ton y = 6.844x R 2 = Henan Sichuan 0.0E E E GDP23 Traffic oil Industrial coal Industrial oil Biofule Traffic oil

MODEL VALIDATION 1.E+00 1.E+05 1.E+001.E+05 1.E+00 1.E+02 1.E+04 1.E+001.E+021.E+04 1.E+00 1.E+05 1.E+001.E+05 Model validation

MODEL UNCERTAINTY 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

GLOBAL EMISSION preliminary Continent/countryEmissionPercentage Total World % Total Asia % Total South and South-east Asia % India % Total East Asia % China % Total Western and Central Asia % Total Africa % Total Western and Central Africa % Total Eastern and Southern Africa % Total Northern Africa % Total North and Central America % Total North America % United States % Total Central America % Total Europe % Total South America % Total Oceania %

VALIDATION USA, 1990 UK, 1995 EU countries- BaP Incineration transportation Aviation ind. Coking Incineration Ind. coal Aluminum

GLOBAL EMISSION DENSITY preliminary

EMISSION vs. GDP and Income Emission density, log(Gg/y) Residual, log(Gg/y) GDP, log(USD)Income, log(USD/y) y = x y = x LgEmission = lgGDP – lgIncome – r 2 = 0.843, n = 168,

SUMMARY Total emission of PAH 16 in China: 116,000 ton in % carcinogenic compounds Major sources: indoor biomass burning, small-scale coke ovens Increased over time Global emission of PAH 16 : 522,000 ton in 2003

33 1.INTRODUCTION 2.EMISSION INVENTORY 3.DISPERSION MODELING IN GUANGDONG 1.INTRODUCTION 2.EMISSION INVENTORY 3.DISPERSION MODELING IN GUANGDONG

METHODOLOGY Spatial resolved emission Potential Receptor Influence Function (PRIF) Forward trajectories (HYSPLIT) Partitioning, degradation, dry/wet deposition 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 ,000 km 2, over 80 million population 60 x 60 km 2 resolution China Guangdong

ANNUAL MEAN OUTFLOW OF PYRENE 2001 Annual mean PRIF (PYR) from Guangdong based on daily trajectory calculation Total PRIF: 5.37x10 -1, 2.56x10 -3 and 8.92x10 -5

SEASONAL VARIATION IN OUTFLOW Summer vs. winter The East Asian monsoons domination

SPECIAL WEATHER CONDITIONS Stagnation (May 7, 2001), typhoon (July 6, 2001), uplifting (Jan. 23, 2001) One day emission, 5 days transport

INTERANNUAL VARIATION PYRENE 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)

MODELING FOR CHINA, PRELIMINARY Forward trajectory, PRIF PRIF of PYR and BaP Resolution: 24 km x 24km x 12 min Euler atmospheric transport model Annual mean conc. at 1.5 m height, log(pg/m 3 coupled with a fugacity multi-media model 1.5, 3.9, 10, 100, 500, 1000, 2000, 3000, 7000 m

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

FINANCIAL SUPPORT NATIONAL SCIENTIFIC FOUNDATION OF CHINA ACKNOWLEDGEMENT