Characteristics and Sources of Particulate Polycyclic Aromatic Hydrocarbons ( PAHs) During Haze Period in Guangzhou

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1 ENVIRONMENTAL SCIENCE Vol. 30,No. 6 Jun.,2009 PAHs 1,2,3, 2,3, 3, 3 (11, ; 21, ; 31, ) : ( ) PM 10, PAHs. PAHs,. [ a ] [1,2,32cd] [ah] [ghi ] [1,2,32cd] [ah] [ghi ], [ a ] [ e ] [ a ]. BEQ ng m - 3,, BEQ ( 2176 ng m - 3 ),. BEQ,., PAHs, PAHs ; PAHs,. : ; ; ; ; :X511 :A : (2009) Characteristics and Sources of Particulate Polycyclic Aromatic Hydrocarbons ( PAHs) During Haze Period in Guangzhou DUAN Jing2chun 1,2,3, TAN Ji2hua 2,3, SHENG Guo2ying 3, FU Jia2mo 3 (11Chinese Research Academy of Environmental Sciences, Beijing , China ; 21Department of Environment Science and Engineering, Tsinghua University, Beijing , China ; 31State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou , China) Abstract :PM 10 (particulates matter with aerodynamic diameter < 10 m) samples were collected at Liwan and Wushan site in Guangzhou city between March 2002 and June Polycyclic aromatic hydrocarbons ( PAHs) were studied during haze and non2haze periods in both summer and winter. PAHs pollution was serious in haze period compared with that in non2haze period, especially in winter. Compared with non2haze period, Phe,Ant,Flu,Pyr,BaA,Chr,IcdP,DahA and BghiP were more abundant in haze period in summer, and BaF,BeP,BaP,Pery,IcdP, DahA and BghiP were more abundant in haze period in winter. The BEQ values were 315 ng m - 3, 3135 ng m - 3, 1143 ng m - 3 and 1310 ng m - 3 in non2haze in summer, in haze in summer, in non2haze in winter and in haze in winter, respectively. The BEQ values in non2haze in summer, in haze in summer and in non2haze in winter in Guangzhou (average : 2176 ng m - 3 ) were relatively low in Chinese cities, and comparable with oversea cities. However, the BEQ value in haze in winter was relatively high in Chinese cities. It indicated that haze in winter would impair human health seriously. The diagnostic ratios suggested gasoline and diesel vehicle emission were main sources of PAHs in summer, and diesel vehicle and coal combustion emission were main sources of PAHs in winter ; PAHs may come from both local sources and long2range transportation in non2haze in winter. Key words :PM 10 ; polycyclic aromatic hydrocarbons(pahs) ; haze ; Guangzhou ; health effect.,,.,. [1 ], [2 ]. Raloff [3 ], [4,5 ]. [6 10 ], ( PAHs) [7 ].,PAHs : ; : : ( ) ; ( ) ; (OGL ) : (1974 ),,,,.

2 6 : PAHs 1575,. PAHs, , (20 m), (25 m),.. Anderson PM 10 (Model GUV2 16HBL), 1113 m 3 min h. (QM2Whatman, 2013 cm 2514 cm), h, % 24 h, , 1 PM 10, 10 :30 10 :30,. 112,, PAHs. 30 ml, 30 min, 500 ml, 3.,,. 110 ml, 014 ml, : 2 ( Plateform, VG ), DB5 (J &W Scientific,30 m 0125 ( ) (8) (7) Πkm mm 0125 m),. : 290, 300, 70 ev ; : 60, 5 min, 3 min , 20 min. :, mπz :50 500, [7 ],. 114 (QAΠQC),. PAHs :D102Acenaphthene 5913 % 9614 %, D102Phenanthrene 6214 % 9815 %, D122 Chrysene 7315 % %, D122Perylene 6317 % %,,,. PAHs : ( Phe, 3 ) (Ant, 3 ) ( Flu, 4 ) ( Pyr, 4 ) (Chr, 4 ) [ a ] (BaA, 4 ) [ b + k ] (BbkF, 5 ) [a ] (BaF, 5 ) [a ] (BaP, 5 ) [ e ] (BeP, 5 ) (Pery, 5 ) [ah ] (DahA, 5 ) [ 1, 2,32cd ] ( IcdP, 6 ) [ghi ] (BghiP, 6 )., US EPA , 20 22, 0. 1,,. SO 2 NO x,,. Table 1 Meteorological conditions during sampling periods in Wushan site Π Π% SO 2 Πm s - 1 Π g m - 3 NO x PM 10 Π g m - 3 Π g m (10) > (6) > PAHs 2 3 PAHs. PAHs ng m - 3, PAHs, ; PAHs ;. PAHs.,,, PAHs.

3 PAHs Πng m - 3 Table 2 Seasonal concentrations of PAHs in Liwan siteπng m - 3 ( ) ( ) ( ) ( ) mean min max mean min max mean min max mean min max Phe Ant Flu Pyr BaA Chr BbkF BaF BeP BaP Pery IcdP DahA BghiP PAHs PAHs Πng m - 3 Table 3 Seasonal concentrations of PAHs in the Wushan siteπng m - 3 ( ) ( ) ( ) ( ) mean min max mean min max mean min max mean min max Phe Ant Flu Pyr BaA Chr BbkF BaF BeP BaP Pery IcdP DahA BghiP PAHs PAHs PAHs. PAHs,. 1, PAHs 3 4 PAHs (10 % 35 %),5 6 PAHs (65 % 90 %), PAHs,. Phe Ant Flu Pyr Chr PAHs Phe Ant Flu Pyr BaA Chr IcdP DahA BghiP, BbkF BaF BeP BaP Pery. BaF BeP BaP Pery IcdP DahA BghiP, Phe Ant Flu Pyr BaA Chr BbkF. PAHs BbkF IcdP, Chr BbkF. 214 PAHs ( diagnostic ratios), PAHs. 4 PAHs.

4 6 : PAHs PAHs Fig. 1 Contributions of individual compounds to the sum of all investigated PAHs at Liwan site 4 PAHs Table 4 Diagnostic ratios of PAHs in PM 10 FluΠ(Pyr + Flu) BaAΠ(BaA + Chr) IcdPΠ( IcdP + BghiP) BaPΠBeP BghiPΠBeP BaPE 1) ) BaPE = BaA BF BaP + DahA IcdP 0108 FluΠ(Flu + Pyr) ,, [11 ].,,,,. BaAΠ(BaA + Chr), , [12 ], BaAΠ(BaA + Chr), ( ),., BaAΠ(BaA + Chr) [13 ]. BaAΠ (BaA + Chr) 1 m , 1 m < 1 m BaAΠ (BaA + Chr), < 1 m. IcdPΠ(BghiP + IcdP) [14 ].,. IcdPΠ(BghiP + IcdP) , PAHs, IcdPΠ(BghiP + IcdP) ,, PAHs., 50 %, IcdPΠ(BghiP + IcdP). BaP,BaPΠBeP PAHs. 2 PM 10 BaPΠ BeP PAHsΠPM 10 4, BaPΠBeP, BaPΠBeP ;,BaPΠBeP. BaPΠ BeP,,BaP ;, BaPΠBeP., ( BaPΠBeP ), ( BaPΠBeP ),

5 PAHs,, Duan [15 ].,BaP ng m - 3, 8164 ng m - 3. BaP, 3164 ng m PAHs [ 11] Table 5 Toxic equivalence factors of PAHs PAHs TEF PAHs TEF BaP 1 Chr 0103 Phe BkF 011 Ant BbF 0105 Flu 0105 IcdP 011 Pyr BghiP 0102 BaA PAHsΠPM 10 BaPΠBeP PM 10 Fig. 2 Comparison between the values of PAHsΠPM 10, BaPΠBeP and PM 10 BghiPΠBeP [16 ], BghiPΠBeP ,,,, IcdPΠ(BghiP + IcdP).,,,. 215 PAHs,, PAHs., PAHs., BaP PAHs ( TEFs) PAHs,, PAHs,Larsen [17 ] BaP PAHs (toxic equivalence factors, TEFs), 5. PAHs BaP, 1 ng m - 3 (WHO), 10 ng m - 3. BaP (BEQ) :BEQ = ( i ) ( i TEF). 5 PAHs PAHs TEF. 6 PAHs BEQ. BEQ ng m - 3, 513 ng m - 3., BEQ ( 2176 ng m - 3 ),. BEQ,. BEQ, BEQ BaP 68 %, BaP,,. 6 BEQ [ 18] Table 6 BEQ level and its contribution in different cities in China and abroad BEQΠng m - 3 BaP Π% [19 ] [20 ] [21 ] [19 ] [22 ] [18 ] BEQΠng m - 3 BaP Π% [23 ] [24 ] [24 ] [24 ] [24 ] [25 ] (1) PAHs 8

6 6 : PAHs ng m - 3. PAHs,, PAHs. (2) Phe Ant Flu Pyr BaA Chr IcdP DahA BghiP, BaF BeP BaP Pery IcdP DahA BghiP. (3) PAHs, PAHs PAHs,. (4) BEQ ,,. BEQ 1310,,. : [ 1 ] Ruzer L, Harley N. Aerosols handbook : measurement, dosimetry, and health effects[m]. CRC Press, [ 2 ] Menon S, Hansen J, Nazarenko L, et al. Climate effects of black carbon aerosols in China and India[J ]. Science, 2002, 297 : [ 3 ] Raloff J. Sooty air cuts China s crop yields [J ]. Science News, 1999, 156 : 356. [ 4 ] Jacobson M Z. Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols[j ]. Nature, 2001, 409 : [ 5 ] Kang C M, Lee H S, Kang B W, et al. Chemical characteristics of acidic gas pollutants and PM 215 species during hazy episodes in Seoul, South Korea[J ]. Atmos Environ, 2004, 38 : [ 6 ],,,. [J ]., 2007,23(1) :126. [ 7 ],,,. PAHs [J ]., 2006, 26(1) : [ 8 ],,,. [J ].,2008,27(3) : [ 9 ],,,. PM 10 [J ].,2005, 25 (7) : [10 ],. [J ]. ( ), 2006, 34(5) : [11 ] Rogge W F, Hildemann L,Mazurek M A, et al. Sources of fine organic aerosol : 2 Non2catalyst and catalyst2equipped automobiles and heavy duty diesel trucks[j ]. Environ Sci Technol, 1993, 27 : [12 ] Kavouras I G, Koutrakis P, Tsapakis M, et al. Source apportionment of urban particulate aliphatic and polynuclear aromatic hydrocarbons ( PAHs) using multivariate methods[j ]. Environ Sci Technol, 2001, 35(11) : [13 ],,,. PAHs [J ]., 2006, 27 (4) : [14 ] Grimmer G, Jacob J, Naujack K W. Profile of the polycyclic aromatic compounds from crude oils2inventory by GC, GC2MS[J ]. PAH in Environmental Materials : Part 3. Fresenius Z Anal Chem, 1983, 316 : [15 ] Duan J, Bi X, Tan J, et al. Seasonal variation on size distribution and concentration of PAHs in Guangzhou city, China [ J ]. Chemosphere, 2007, 67 : [16 ] Nielsen T. Traffic contribution of polycyclic aromatic hydrocarbons in the center of a large city[j ]. Atmos Environ, 1996, 30 : [17 ] Larsen J C, Larsen P B. Chemical carcinogens[ A]. In : Hester R, Harrison R. Air pollution and health [ C ]. Cambridge, UK: The Royal Society of Chemistry, [18 ],,,. PM 10 PAHs BEQ [J ]., 2006, 25 (3) : [19 ],,,. [J ]., 2002, 22 (3) : [20 ]. (PM 10, PM 215 ) [D]. :, [21 ],,,. (PAHs) [J ]. ( ), 2004, 43 (6) : [22 ] Guo H, Lee S C, Ho K F, et al. Particle2Associated Polycyclic Aromatic Hydrocarbons in Urban Air of Hong Kong [ J ]. Environ, 2003, 37 : Atmos [23 ] Takeshi O, Takashi A, Masahiro F, et al. Spatial Distributions and Profiles of Atmospheric Polycyclic Aromatic Hydrocarbons in Two Industrial Cities in Japan[J ]. Environ Sci Technol, 2004, 38 : [24 ] Halsall C J, Coleman P J, Davis B J, et al. Polycyclic Aromatic Hydrocarbons in U. K. Urban Air [J ]. Environ Sci Technol, 1994, 28 : [25 ] Smith D J T, Harrison R M. Concentrations, Trends and Vehicle Source Profile of Polynuclear Aromatic Hydrocarbons in the U. K. Atmosphere[J ]. Atmos Environ, 1996, 30 (14) :