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Gas/Particle Partitioning of Polycyclic Aromatic Hydrocarbons in the Spring of Beijing, China Xiaoxi Liu EAS 6410, Spring 2012.

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Presentation on theme: "Gas/Particle Partitioning of Polycyclic Aromatic Hydrocarbons in the Spring of Beijing, China Xiaoxi Liu EAS 6410, Spring 2012."— Presentation transcript:

1 Gas/Particle Partitioning of Polycyclic Aromatic Hydrocarbons in the Spring of Beijing, China Xiaoxi Liu EAS 6410, Spring 2012

2 Summary Introduction Sampling and Analysis Results and Discussion - PAHs concentrations - Assessment of three gas/particle partitioning models Conclusions

3 PAHs and Gas/Particle Partitioning Polycyclic aromatic hydrocarbons (PAHs): organic compounds arranged in two or more aromatic rings Human Health: carcinogenic, mutagenic, teratogenic Benzo(a)pyrene Gas/particle partitioning influencing their fate (long-range transport, transformation, and removal mechanism) Many efforts have been devoted to study the particulate concentrations of PAHs, not many to Gas Controlling air quality needs concurrent study of gas and particle phase PAHs

4 Sampling Dingling Dongsi Yizhuang Gucheng April 1, 8, 14, 20 and 26, 2011. 0:00-24:00 Beijing, China

5 Analysis 16 EPA priority PAHs: Gas chromatography – mass spectrometry (GC- MS) Quality control: calibration curve, recoveries, detection limits Measurement of Organic Carbon/Elemental Carbon: Thermal-Optical- Transmittance (TOT) analysis method NAP ACY ACE FLU ANT PHE FLT PYR CHR BaA BbF BkF BaP IND BGP DBA

6 Results and Discussion – PAHs Levels PAH particle-phase gas-phase DinglingGuchengDongsiYizhuang DinglingGuchengDongsiYizhuang NAP0.310.960.690.296.4722.9710.7712.49 ACYN.D. 0.16N.D. ACEN.D. 0.713.901.411.31 FLU0.691.080.810.645.8116.949.7312.08 PHE1.912.751.922.1012.6039.0925.2831.87 ANT2.281.531.821.161.182.951.772.49 FLT3.114.522.754.183.078.765.988.69 PYR2.643.752.243.761.835.533.695.88 BaA2.022.901.902.691.261.691.211.46 CHR1.603.661.813.070.150.450.490.75 BbF4.297.954.817.310.581.110.470.60 BkF0.921.930.951.75N.D. 0.040.01 BaP2.203.241.973.23N.D. IND4.176.364.456.00N.D. DBA0.731.780.711.83N.D. BGP2.634.562.954.34N.D. 16 PAHs 29.4946.9629.9442.3434.84107.6363.3180.37 ng/m^3

7 Partitioning Mechanisms Physical adsorption onto the particle surface Absorption into the organic matter of aerosols Gas-particle partition coefficient, K p (m 3 /ug ): F (ng/m 3 ) -particle concentration of PAHs A (ng/m 3 ) -gas concentration of PAHs TSP - concentration (ug/m 3 ) of the total suspended particles Emitted PAHs Active sites Organic matter Adsorption Absorption Both mechanisms lead to a linear relationship between logK p and the log of the PAH subcooled liquid vapor pressure (logp L 0 ): Ideally, under equilibrium conditions, the slope should be equal to 1

8 The logKp-logp L 0 Relationship Dingling Gucheng DongsiYizhuang Slope m r Intercept b r LocationsSitesminmaxmeanminmaxmeanR2R2 References Beijing /China Urban& Suburban -0.46-0.25-4.02-2.980.59-0.87 present study Beijing /China Urban-1.45-0.90-1.28-6.16-4.97-5.61 0.57(Spring) 0.73(Annual) Wang 2011 Guangzh ou /China Urban-0.86-0.46-0.64-6.090.85Yang,2010 Suburban-0.79-0.45-0.63-5.960.86Yang,2010 Petrana /Greece Continental background -0.48-0.23-0.32-3.38-1.98-2.750.65Terzi,2004 Athens /Greece Urban-1.49-0.16-6.50-3.20 Sitaras,200 3 The partitioning of PHE, ANT, FLT, PYR, BaA, CHR was studied

9 Partitioning Models 1. Junge-Pankow Adsorption Model calculated from K p and TSP: - the fraction of PAH sorbed to particulate matter 2. K OA Absorption Model K OA - octanol–air partition coefficient 3. K OA – K SA Model: the dual organic matter absorption model combined with the soot carbon adsorption model K SA - soot–air partition coefficients

10 Assessment of Junge-Pankow Model The Junge–Pankow model underestimated the particulate sorption of PAHs Other absorption partitioning mechanisms in addition to surface adsorption

11 Assessment of K OA & K OA -K SA Models

12 Adsorption onto soot is more important for PAHs with lower molecular weight.

13 Conclusions The average total PAH concentrations were 64.33 ng/m 3, 154.59 ng/m 3, 93.25 ng/m 3 and 122.71 ng/m 3, at Dingling, Gucheng, Dongsi, Yizhuang Lighter PAHs are found predominantly in the gas phase, while those with four or more rings are found mainly in the particle phase The regression slopes of logK p versus logp L 0 were much shallower than -1, suggesting non-equilibrium partitioning The Junge–Pankow adsorption model and K OA model both under- predicted experimental K p. However, in general the dual model fit our experimental K p well, suggesting that PAHs adsorption onto soot carbon and absorption into organic matter were both important for PAHs gas/particle partitioning in Beijing

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