Availableonlineatwww.sciencedirect.comScience directNTALJournal of Environmental Sciences 2010, 2207)1014-1022Characterization of polycyclic aromatic hydrocarbons and gas/particlepartitioning in a coastal city, Xiamen, Southeast ChinaJinping Zhao, Fuwang Zhang. 2, Jinsheng Chen,, Ya Xul.21. Key Laboratory of Urban Environment and Health, institute of Urban Emvironment, Chinese Academy of SciencesXiamen 361021, China. E-mail: jpzhao@ iueaccn2. Graduate School of Chinese Academy of Sciences, Beijing 100049, ChinaReceived 22 June 2009; revised 07 January 2010, accepted 26 January 2010AbstractAn intensive sampling program had been undertaken in autumn(October, 2008)and winter(December, 2008 and January, 2009)at urban(Xiamen University and Xianyue residential area), suburban(Institute of Urban Environment), industrial area(Lulian Hotel)and background (Tingxi Reservoir) in Xiamen, Fujian Province, to characterize the atmospheric concentration and gas-particle phasepartitioning of PAHs. The average concentration of total PAHs in winter was almost 1.7 times higher than those in autumn. The logscale plot of Kp versus sub-cooled liquid vapor pressure( PD) for all the data of autumn and winter season samples gave significantlydifferent slopes. The slope for the winter samples (-0. 72 )was steeper than that for the autumn samples (-0.58). The partitioning resultsindicated that slope values varied depending on characteristics of specific site, source region and meteorological conditions whichplay important roles in the partitioning of PAHs. In addition, local emission sources had a stronger effect on partitioning results thanlong-transported polluted plume. The sources of PAHs in five sampling sites in Xiamen also have been discussed initially Diagnosticratios showed that the primary source of PAHs in urban, suburban and industrial area was from vehicle exhausts. while emission frompetrochemical factory and power plant was another main contributor to industrial area.Key words: PAHs; gaseous/particulate partitioning: diagnostic ratio; XiamenDol:10.1016S10010742(09)602126Introductioncess of environmental cycling (Lammel, 2009; Simcik etal., 1998), which is the key to understand the distlycyclic aromatic hydrocarbons(PAHs)are a large transport pathways and environmental fate of atmosphericgroup of organic compounds composed of at least two PAHs. Although gaseous/particulate distribution of PAHsaromatic rings fused together. These compounds are per has been well documented Vardar et al., 2004; Lammelstent organic pollutants exist in environment extensively. 2009), the process of PAHs in gaseous/particulate partiSome PAHs are considered to be mutagenic and/or car- tioning is still not understood completely( Galarneau etisogenic compounds and are linked to health problems, al., 2006). It is therefore essential to analysis semi-volatilesuch as cataracts, kidney and liver damage. Thus, they have PAHs behavior in air, especially for Xiamen where noattracted a significant amount of attention in recent years literature has reported partitioning of PAHs in gas-and(Dong and Lee, 2009)PAHs are formed during incomplete combustion of Xiamen, a subtropical city in southeastern China, hasorganic materials from sources, such as residential heating, warm weather and high relative humidity throughoutvehicle exhausts, industrial power generation, and produc- the year(temperature is in the range of 4-38 C; withtion of coal tar. Among various anthropogenic sources of 209C on annual average in 2008). The prevailing windPAHs, the traffic source has been known to be the greatest direction is northeast in autumn and winter, which cancontributor in many countries( Benner et al., 1989; Ye bring air masses to move across northern cities. Xiamenet al., 2006). However, up to now no quantitative source administrative area, with an area of 1565 km and pop-apportionment has been made for atmospheric PAHs in ulation about 2.5 million in 2008, is a main economicamen, Fujian, China and the seasonality of the potentiaV凵中国煤化工sources remains unknownindicment in Xiamen wasGaseous/particulate portioning for semi-volatility and favoCNMH Go06) However, withpersistence of PAHs has an important significantly in pro- the rapid urbanization and industrialization, especiallythe increase of motor vehicles, environment pollutionsCorresponding author. E-mail: jschen @iueaccnmay contain large amount of carcinogenic and mutagenicNo. 7 Characterization of polycyclic aromatic hydrocarbons and gas particle partitioning in a coastal city, Xiamen, Southeast Chinaorganic matter, of which PAHs in total suspended particles petrochemical factory and power plant are located. XY(TSP)were included. Therefore, the inhabitants experience and XU as the urban sampling sites are represent differenta considerable increase of adverse health effect, which functional areas. the former represents commercial areainterested people' s concern.where traffic road and residential buildings are surrounded,Although PAHs in Xiamen have been reported in some while the later represents educational area which is nearpublications(Ye et al., 2006), no intensive research has seaside, street and temple of Nanputuo. The sampling sitesbeen conducted in Xiamen on PAHs level in the atmo- were placed on the rooftop of residential building andsphere, especially for the distribution of PAHs in gas- teaching building, about 15 and 18 m above the ground,and particle-phases. There is a lack of information abouPAHs occurrence in the atmosphere in Xiamen. Therefore,The air samples were collected simultaneously fromthe objectives of this article were:(I)to provide ambient every two sites during 23-31 October, 2008(representPAHs concentration in gaseous and particulate phases, as autumn) and 24 December 2008 to 5 January 2009(rep-well as to describe the gaseous/particulate partitioning in resent winter). Air samples were collected every 24 hr.atmospheric aerosols during autumn and winter; and (2 )to An Andersen high-volume sampler model PS-1(Thermoidentify possible sources of PAHs in this coastal cityFisher Scientific, USA)with flow rate of 160 L/min wasused for collecting suspended particles onto a filter, while a1 Experimentbackflow adsorbent trap retained the gas fraction of PAHs.Particles were collected by passing air through Whatman1.1 Sampliglass fiber filters(GFF, 10.16 cm diameter). The adsorbentcartridge used was polyurethane foam (PUF, length 8.0 cm.Air samples were collected from five sites in Xiamen: diameter 6.25 cm)to collect PAHs in gas-phase. The GFFsTingxi Reservoir(TX), Institute of Urban Environment were previously annealed for 5 hr at 450C in a furnaceCAS(TUE), Lulian Hotel(LL), Xianyue Residential Area to remove organic matter and PUFs were pre-cleaned(XY), Xiamen University (XU)(Fig. 1)TX is a background and located in forestry mountainby dichloromethane (DCM)in Soxhlet for 72 hr, afterprocessed, these sampling materials were stored in bakedarea with a medium-sized reservoir. The sampling site was aluminum foil within sealed polyethylene plastic bagstaken on the rooftop of the reservoir office, approximately before use. After sampling, loaded GFFs were wrapped6 m above the ground. IUE as a suburban sampling site with prebaked aluminum foils and sealed with doubleis surrounded by highway, schools, residential buildings layers of polyethylene bags, and PUFs were placed inand Xinglin sea bay. The sampler was placed on rooftop solvent rinsed glass jars with aluminum foil-lined lids, andof laboratory building, about 35 m above the ground. LL then transported to the laboratory and stored at-20oC untilis chosen in an industrial area. The sampler was sited on extraction. All of those filters were weighted before andthe rooftop of a four-story hotel, about 12 m above the after sampling with an analytical balance(Sartorius T-1 14,ground. This sampling site is close to industrial base where Germany)after stabilizing under constant temperature(25±1)° and humidity(50±1)% to get mass concentrationAnxi Counof particulate matter1.2 Analytical procedureStandards of 16 PAHs in a mixture (as specified inUS EPA Method 610)and a surrogate of acenaphthene-Tongan Disterictdyo, phenanthrene-d10, chrysene-d12 and perylene-du2 wereobtained from Ultra Scientific Inc, USA. An internal stan-dard of pyrene dio were obtained as liquid of 99.5% purity(Labor Dr. Ehrenstorfer-Schefers, Germany). All reagentsXianganincluding n-hexane and DCM were chromatogram gradeand purchased from Tedia, USA, which are 95% and99.5% purity, respectivelyJimei districtPUF samples were Soxhlet extracted with DCM for 72hr, while GFFs were extracted with dCm by ultrasonicagitation(KQ300DE, Kunshan Ultrasonic Instrument Co.,Ltd, China). The procedure repeated three times, andeach for 30 min. These extracts were concentrated andthe solvent was removed using rotary evaporator(RE-52AAty Instrument Co.,Siming DistrictLtd中国煤化工tivatedCNMHGmI and the targetFig1 Location of the five sampling sites (TX, IUE, LL, XY, XU) in proximately 1-2 mL. Then, the final volume was adjustedXiamento I mL by nitrogen blowdown and stored in refrigerator atJinping Zhao et al-20oC until analysisambient air was ranged from 5.54 (TX)to 76.55 ng/m3The samples were analyzed with a gas chromatography- (XY) in autumn, and 35.95(XU) to 62.85 ng/m(LL)mass spectrometry (GC-MS) system consisting of an in winter. Table 1 shows that PHE, FLA and PYr wereAgilent model 7890A GC and an Agilent model 5975 mass the dominant congeners among the total PAHs not only inselective detector(MSD)(USA). The MSD operated in particle-phase but also in gas-phase at five sampling siteselectron impact mode with electron energies of 70 eV. A The total concentration of PHE, FLA and PYR rangedcapillary column(HP-5MS UL, 30 m x 0. 25 mm x0. 25 from 0.77(TX) to 37 18 ng/m(XY), 0.43(TX)to 10.14um, length x ID x film thickness)was used. Splitless mode ng/m(XY) and 0.32(TX)to 6.05 ng/m3(XY)in thewas applied at the gC inlet for the introduction of Iautumn samples, respectively, the concentrations of whichsample. The GC temperature was held at 50C for 1 min were higher in autumn than that in winter. Total PAHsand raised to 200C at 10.C/min, then to 280 C at 5C/min concentration in TX autumn and winter samples were 5.54and held for 12 min. The MSD was run in selected ion and 37 37 ng/m, which were lower than those in otherand processing were controlled by a HP Chem-Station data from biomass combustion and temperature inversa urcemonitoring mode for optimum sensitivity Data acquisition sampling sites indicating the influence of pollutionIdentification of individual PAHs was based on thole 1 also indicates that concentration of PAHs in winretention times of target ion peaks(within t 0.05 min of ter were higher than that in autumn and which were alsothe retention of the calibration standard)higher in urban than that in suburban and background. LowThe PAHs determined in this study are abbrevi- levels of photochemical degradation and limited mixtureated as follows: naphthalene(NAP), acenaphthylene layers or the frequent formation of a temperature inversion(ACY), acenaphthene(ACE), fluorene(FLO), henan- layer in the atmosphere in Xiamen during winter wouldthrene(PHE), anthracene(ANT), fluoranthene(FLA), aggravate the occurrence of high PAHs concentration inpyrene(PYR), chrysene(CHr), benzlalanthracene(BaA), the samples. High levels of photochemical degradationzo[b]fluoranthene(BbF), benzo[k]fluoranthene(BkF), and of mixture layers in the atmosphere and frequentbenz[a, h]anthracene (DahA), benzo[a]pyrene( BaP), monsoon and rainfall during autumn would lead to lowindeno[1, 2, 3-cd]pyrene (ledP) and benzolghi]perylene concentrations of PAHs in the samples. The different(BghiP)concentrations of pahs in fiv1.3 Quality assurance and quality controlrelate with surrounding environment. xY was located inresidential areas, which was a commercial area with aField blanks that accompanied the samples from the busy transportation. The dual impacts of vehicle exhaustsampling sites were used to determine any potential and cooking emission may result the highest level con-background contamination during sampling, transport, centration in autumn. LL was placed in industrial district,and storage. Method blanks(solvent)and spiked blanks exhaust from petrochemical factory and power plant was(standards spiked into solvent) were also used. Surrogate the main source of PAHs, and led to the high concentrationstandards were added to all samples (including those of PAHs. Infrastructure construction and agricultural ac-for quality assurance) to monitor procedures and matrix tivity were the main factors which would influence PAHseffects. The blank levels were less than 6% of the mass concentration in IUE. xU was an education and touristin the samples. PAHs level in solvent blanks(n= 5)were area, vehicular emission and the exhaust gas from shipslower than those in the field blanks. The relative difference were sources for PAHs. TX sampling site was surroundingfor individual PAHs congener identified in paired duplicate by forest and a reservoir. There was almost no pollutionsamples were all 13%.source excluding occasional biomass combustion, whichDuring GC-MS analysis, response factors for individual would cause a low concentration of PAHsPAHs relative to the internal standard were determinedThe total particle-phase PAHs in the atmosphere rangedfrom the analysis of the calibration solution containing from 3. 14(TX) to 7 49 ng/m(LL) in autumn samples and16 PAHS, 4 deuterated PAHs and one internal stan- 13. 26(TX)to 23 27 ng/m(XU)in winter samples, whichdard. No any targeted PAHs was detected in standards accounted for 7. 27%(XY)56.73%(TX)and 33.51%or blanks. Analytical recoveries of the surrogate PAHs (LL-64.74%(XU)in the total PAHs, respectively( Figin samples were 48.45%-66.57% for acenaphthene-dIo; 2). Whereas, the total gas-phase PAHs has a higher percent43.60%-64.12% for phenanthrene-d1o: 55.61%101.76% in total PAHs during autumn(43. 27%(TX)-9273%(XY)for chrysene-d12 and 59.90%0-116.05% for perylene-dy2. than that during winter(35.26%(XU)66.49%(LL). ThReported concentrations were corrected for blank levels relationship of distribution of particle /gas-phase PAHsbut not for surrogate recoveries.and temperature can be found in Fig. 2 clearly, where therelative concentration of gas-phase PAHs in autumn were2 Results and discussionhigher than that in winter. This can be interpreted as thegas-particle distribution of semi-volatile PAHs, which was2.1 Ambient air PAH concentration and distribution中国煤化工 PAHs distributionsin winter(GigliottiThe average concentrations of PAHs in particle- and et alCNMHGgas-phase at five sampling sites are shown in Table 1. Figure 3 shows the variations of total PAHs in particle-The total(particle-and gas-phase)PAHs concentration in /gas-phase and concentration of TSP in five sampling sitesNo. 7 Characterization of polycyclic aromatic hydrocarbons and gas/particle partitioning in a coastal city, tSoutheast china1017Table 1 Average concentration of particle- and gas-phase PAHs at five sampling sites(ng/m)Sampling siteTX XUXY(n=4)(n=4)39±005033±002034±003033±001041±006023±02039±00043±002036±009012001±10生00102±O20±00129±003士01±000003±00003030100.17±002031±0.100.62±0.60±0.09185±0±0.12025±0.l1028±0090210.1086±0.48209g0.4139±3.21±0.179±02320±193244±1.78±016005±0011.52±1,17242±1.65144±0.12245±035±060±243±05041±0220±1502035±002024±0156±004086±031029±006040±011.15±0.32±1.03261±156271±1.04347±21Total particle749±1.71449±1473.14±0.893.00±10556±0062106±1452036±25313.26±1872327±6051772±879058±003031±0.11072±0.09088±0.14566±213057±0.00063±002141±006042±0.11053±025109±0813±00±01705061±0.11405±132t12102014±215743±0.130.20008±0000.30±t1.58±030033±065±1.10203±983±25:土土士土士土主土±士6:0m0:00008:00000006±003002±0.02001±00001±0005±0.11D的D003±001001±001Lase PAHs1506±3.12102218240±032824±1457099713419±2381713±2321111431268±1362454±006as avcrage t sD, Rato was obtained by the total concentration of every compounds. ND not detected.a Particle-phaseGas-phaseTemperature24ALL AIUE ATX AXU AXY WLL中国煤化工Flg. 2 Relationship of distribution of total particle-/gas-phase PAlCNMHGIt is obviously that the variation trend of concentration for trend between PAHs in gas-phase and TSP, especiallyPAHs in particle-Phase and TSP was coincident in different that in winter samples. Therefore, there was no significantsampling sites, whereas it was not coincident variation relationship can be found between the concentrations ofJinping Zhao et alC Particle-phase -Gas-phase -+ TSP(4.99%(XY)-26.64%(TX)in autumn and 12. 20% (LLh25.93%(XU) in winter), and PYR(1.49%(TX-1154%E58(UE)in autumn and 4.83%(TX)-1209%(Y)in winter),Autumnand five-to six-ring PAH compounds(Mw 250-300)witl175- low vapor pressure were predominant in the particulatePAHs, including BbF, BghiP, IcdP, BaP, and BkF. Fourring compounds(MW 228)like BaA and CHR had similarconcentrations at some samples in the gaseous and par≌20ticulate phases. PAHs with different molecular weights75have different particulate/gaseous distribution coefficientsthe gaseous phase contribution generally decreased withincreasing molecular weight from 99. 2% to < 0.01%.Fig3 Variations of particle-/gas-phase PAHs and total suspended Two-and three-ring PAHs were associated primarily withparticles (TSP)in five sampling sites.the gaseous phase, 5.and 6-ring PAHs were associatedmainly with particulate phase( Fig 4). These results werePAHs in gaseous phase and TSP. Seasonal trend was consistent with other studies(Bi et al., 2003).In additionapparent for PAHs concentration in gaseous phase. The Fig. 4 also shows the relative composition of PAHs inrelative percent of concentration levels in autumn was high sampling site, excluding background(TX) sampling sites,and gradually decreased in winter. Gustafson and Dickhut has a good consistency, which suggested the PAHs in(1997)suggested that gaseous PAHs(PHE, ANT, FLA, different functional areas have the same or similar sourcesand PYR)have an exponential increase under high ambient of pollutant. Using concentration of 16 class PAHs thattemperature For particulate PAHs, the variation trend of have been detected in suburban sampling sites(IUE)andrelative percent concentration was observed in the opposite other sampling sites(LL, XU, XY and TX)to analysisdirection, with lower relative percent concentration levels correlation(Fig. 5), there was a significant correlation(Pin autumn and higher levels in winter. That was not para- 0.01), excluding TX samples, which further indicated thatthere were similar sources of PAHs in different functionaland frequent formation of a temperature inversion layer inthe atmosphere during winter would deteriorate pollutionof PAHs, and the temperature would affect different rela- 2.2 Comparison of PAHs concentrationstive percents of particle-/gas-phase PAHs, which also can Table 2 displays the PAHs concentration of North Amer-be proved by Fig. 2.ica, Europe, and Asia. From Tables 1 and 2, we can observeFigure 4 shows the distribution of 2-6 ring PAHs in that the average total PAHs concentration in winter wasparticle-and gas-phase The predominant PAHs in the gas. about 1.7 times higher than those in autumn.This differentphase were two- to four-ring compounds, including PHE might be explained by the fact of meteorological factor,( 25.27%(TX)-5209%(XY)in autumn and 25.92%(TX] such as frequent temperature inversion would aggrandize48.18%(LL)in winter), FLA(2.88%(TX)19.86%(UE) PAHs pollution in winter. The average total PAHs con-in autumn and 9.92%(TX-1918%(IUE)in winter), FLo centration in autumn was similar with that in Houston:2.Ring [3-Ring DOWXYATXWXUWIAIUE中国煤化工ALLCNMHFig.4 Distribution of 2, 3,4,5, 6-ring PAHs in particulate and gaseous phases. A: autumn; w:winter.Characterization of polycyclic aromatic hydrocarbons and gasparticle partitioning in a coastal city, Xiamen, Southeast ChinaAutumnwinter▲XUR2=095▲汤曾XYR2=091Concentration of 16 class PAHs in IUE(ng/m2)Concentration of 16 class PAHs in IUE (ng/m)Fig. 5 Correlation of the concentration of individual PAHs in IUE and LL/XU/XY / TXTable 2 Comparison of total PAHs concentration between the present 2.3 Gas-particle partitioning of PAHsstudy and previous publicationsLocationGas-particle partitioning of PAHs is subjected to sea-(ng/mysonal variation not only because of changes in emissionLondon, UKprofiles but also in meteorological conditions and particleLondon, UKDimashki et al.. 2001characteristics. In many studies, using Eq.(1), the gas-Chicago, USA4499particle partitioning of PAHs(Kp)has been examined asa function of sub-cooled liquid vapor pressure(Po )of thecompounds(Fernandez et al., 2002; Esen et al., 2008)2000-200279=m院Pinto et al. 1998oronto, CanadaFocusing on a single sampling period reduces the effectong Kong, Chinaof fluctuations in atmospheric conditions and particlecharacteristics. Liang et al.(1996)suggested that underGuo et al. 2003equilibrium conditions and for the same compound classaliguan, China 200Cheng et al, 2006the slope (mr)should be -l regardless of whether ab-Xiamen, Chinasorption or surface adsorption dominates the partitioningprocess. However, in more recent studies it was concludedthat mr may deviate significantly from-I for equilibriumpartitioning(Vardar et al., 2008; Bi et al., 2004). The de-Naumova et al, 2002)and Kozani (Terzi and Samara, viations from the equilibrium value of-1 have commonly2004), in winter was similar with that in Birmingham, been attributed to sampling artifacts, non-exchangeabilityUK(Harrad and Laurie, 2005)and lower than Chicago new pollutants input during sampling and a lack of con-(Simick et al., 1997; Sun et al., 2006), Teplice(Pinto et stancy in activity coefficients(Terzi and Samara, 2004;al.,1998). Compare with the coastal city in China, we Vardar et al, 2004; Goss and Schwarzenbach, 1998; Sim-than other coastal city from north( Qingdaole was lower cik et al. 1998). The effects of non-exchangeable PAHsPAHs pollution in Guangzhou was serious in these coastal significantly large due to the facts that they are mainlycities, where the PAHs concentrationlywas approximateladleman, 1992). In10 times higher than that in Xiamen. In addition, it a word, if the activity coefficient of the chemical in thwas obvious that PAHs concentrations in Xiamen dunng organic matter is not constant, it is also possible to getautumn and winter were higher than that in WaLiguan slopes not equal to-1which is a typical background site and only has 19 ng/m? Figure 6 shows that the slope for the autumn samplesin ambient atmosphere( Cheng et al. 2006). However, the was-0.58, whereas it was -0.72 for the winter samples,average value of PAHs in background (TX, 21. 4 ng/m) which indicated that the winter samples to be closer towas slightly higher than that in Waliguan. In a word, the equiliaverage PAHs concentration in Xiamen was low compared partick中国煤化工umn samples. Gaswith other coastal cities among China, North America and in thiland winter samplesEurope. Nevertheless, it is worth of, for administrative from uroC N MH Ghe results obtainedLaxen in ue guangzhou City by Bipartment, paying attention to atmospheric pollution, in et al. 2004), in Houston by Naumova et al. (2003)and inorder to keep a better environment of this tourism-cityTurkey by esen et al. (2008). For an urban area, similarJinping Zhao et al.vl.22▲ Autumn y=-058X-401R2=053affect partitioning coefficient of PAHs. CharacterizationWinter Y=-072X-460R2=0.6of the organic matter associated with gaseous/particulatepartitioning of PAHs must be done to support this interpretation(Offenberg and Baker, 2000). Of course, detailedinfluencing factors at each site need to be studied deeply toexplain the differences on those partitioning results2233Based on these observations it can be concluded thatspecific characteristics of sampling sites and meteorological conditions play important roles in the gas-particlepartitioning of PAHs in Xiamen.2.4 Primary research on sources of PAHs in five sam-Atmospheric PAHs profiles can be affected by me-teorological variables such as sunlight radiation andFig6 Plots of logk, versus logPl for all the samples collected in temperature, and its sources mainly come from incompletXiamen. Data source of logP is from Offenberg and Baker(1999).combustion. Despite these facts, the ratios between someof these compounds were considered as"fingerprint"ofresults have been reported(Esen et al., 2008: Terzi and an emission source(Khalili et al., 1995; Dickhut et alSamara, 2004: Lohmann et al., 2000). Lohmann et al. 2000), and this ratio was diagnostic parameters(diagnostic(2000) observed steeper slope(0.77)for coldest event ratios). These diagnostic ratios between PAHs were usedand shallowest slope (0.67)during warmest event in the to characterize potential emission sources and distinguishnorthwest England atmosphere On the other hand, in some PAHs sources(Kavouras et al., 2001).studies opposite seasonal pattern was observed, slopes in Table 1 provides information on diagnostic ratioswinter period were shallower than those in summer period for PAHs, such as FLA/(FLA+PYr), BaN/(BaA+CHr),(Galarneau et al., 2006). It is worthy to note that not all of BaA/(BaA+CHR)and IcdP/(IcdP+BghiP), which can bethe studies showed same kind of seasonal trend in slopes. used to investigate their origin or as an indication ofIt has been reported that partitioning of PAHs showed the aging of air samples(Lohmann et al., 2000). Adifferent characteristics depending on air mass trajectories comparison between the various diagnostic ratios by US(Vardar et al., 2004, 2008). Figure 7 shows backward EPA (2003), Yunker et al. (2002)and Pio et al. (2001)trajectories of air masses coming from northeast areas was conducted. Analysis of the ratios could be associatedto sampling site in Xiamen, and also indicates that the to various sources. Because only TSP may result in ainfluence of wind direction in autumn and winter is al- significant underestimation of the contribution of anthro-most same. However, it was possible that the pollution pogenic emission, these ratios were determined by thecontributed to Xiamen would be different during autumn total concentration including the gaseous and partand winter, and carried much more organic matter by air phases. In particular, the FLA/(FLA+PYR) valuesmass from the Yangtze River Delta in winter which may determined to be 0.57 and 0.63 in ATX and WTx,tYH中国煤化工CNMHGAutumnFig 7 Backward trajectories of air mass from northeast to Xiamen during sampling timesNo.7 Characterization of polycyclic aromatic hydrocarbons and gas/particle partitioning in a coastal city, Xiamen, Southeast Chinaare comparable to the values reported for biomass (wood indicated that vehicle exhausts were a primary source foror vegetation) combustion(0.51 0 16)(Yunker et al. PAHs in different functional areas of Xiamen. In addition,2002: Pio et al., 2001: US EPA, 2003). The source of coal combustion was another main source in industrialbiomass combustion for TX can be further assessed from area. Therefore, it can be proposedat some effectiveIcdP/(IcdP+BghiP)ratios(0. 42+0.18)by Yunker et al. control measures should be taken to reduce the(2002), which was coincident with results of this study atmospheric pollution and keep the reputation ofrt①(0.51 in ATX and 0.50 in WTX). The literature reported environment for Xiamen City, China.values for IcdP/(IcdP+ BghiP)are 0.36+ 0. 14 and 0. 48*0.29 for oil and coal combustion, respectively (Yunker Acknowledgmentset al., 2002; US EPA, 2003). The mean ratio in this study This work was supported by the Knowledge Innova-was 0.44-0.48 in urban and industrial area, respectively, tion Program of the Chinese Academy of Sciences(Nowhich is comparable to that for vehicle emissions and KZCX2-YW-422-4), the Fujian Natural Science Foun-exhausts form petrochemical factory and power plant. dation for Young Scientists(No. 2009J05104)and thehe BaA/(BaA+CHR)ratio in WXU and AXY was 0.68, Program of Science and Technology Bureau of Xiamenindicating that diesel vehicle was a great contributor in (No. 3502Z20081117). The authors would like to thank Dr.these areas and also can be assessed by PHE/(PHE+Ant) Xian Zhang and Dr. Youwei Hong for technical assistancethat was 0.73+0.18 in literature(Yunker et al. 2002; US and GC-Ms data acquisition. Anonymous reviewers areEPA, 2003). The parameters were compared with those thanked for their commentsreported previously(Yunker et al, 2002; Pio et al., 2001US EPA, 2003). Figure 5 also approves indirectly there Referenceshave similar sources in these sampling sitesOverall, our results suggest that the major source of Benner B A, Gordon GE, Wise S A, 1989. Mobile sources oforganic compounds in the air of urban and industrialatmospheric polycyclic aromatic hydrocarbons: A roadwayarea in Xiamen was fossil fuel combustion from automo.tunnel study. Environmental Science and Technology, 23(10)biles. The ratios of FLU/(FLU+PYR) was determined by1269-1277Rogge et al.(1993)for non-catalyst(0.41), and catalyst- Bi xH, Sheng G Y, Peng P A, Chen Y J, Zhang ZQ,Fu JM2003. Distribution of particulate-and vapor-phase n-alkanesequipped (0.51)automobiles. The ratio was calculated toand polycyclic aromatic hydrocarbons in urban atmosphere ofbe 0.60-0.63 in this study, which is close to the value fcGuangzhou, China. Atmospheric Environment, 37(2): 289-298catalyst-equipped automobiles. In Xiamen City, in order Bi X H, Sheng G Y, Tan J H, Tang X L, Fu J M, 2004. Phasto keep favorable place for living, most of automobilesartitioning of polycyclic aromatic hydrocarbons(PAHs )in theare equipped with the converters after 2000. In addition,atmosphere. Acta Scientiae Circumstantiae, 24(1): 101-106emission from coal combustion in power plant was another Cheng H R, Zhang G, Liu X, Li I, Qi S H, Zhao Y C,2006main source for industrial areaStudies on polycyclic aromatic hydrocarbons in the atmospherealiguan, Qinghai. China Environmental Science, 26(6):6466493 ConclusionsDickhutR M, Canuel E A, Gustafson K E, Liu K, Arzayus K M,Walker S e et al. 2000. Automotive sources ofThe total particle-phase PAHs in the Xiamen atmo-polycyclic aromatic hydrocarbons associated with particulatesphere ranged from 3. 14 (TX)to 7.49 ng/m'(LL)inmatter in the Chesapeake Bay Region. Environmental Scienceand Technology, 34(17): 4635-4640autumn and 13. 26 (TX) to 23 27 ng/m(XU) in winter, Dimashki M, Lim L H, Harrison R M, Harrad S, 2001. Temporaland the total gas-phase PAHs in the air between 2.40trends, temperature dependence, and relative reactivity of at-(TX)and 71.00 ng/m(XY) in autumn and 12.68 (XUmospheric polycyclic aromatic hydrocarbons. Emvironmentaland 24.54 ng/m(XY) in winter. PHE, FLA and PYRScience and Technology, 35(11 ): 2264-2267were the predominant compounds in Xiamen. Measured Dong T T, Lee B K, 2009. Characteristics, toxicity, and sourceatmospheric PAHs concentration showed that the relativeapportionment of polycyclic aromatic hydrocarbons(PAHs)inconcentration of particle-phase was significantly lower inroad dust of Ulsan, Korea. Chemosphere, 74(9): 1245-1253autumn samples than that in winter samples, which was Esen F, Cindonuk SS, Tasdemir Y, 2006.Ambient concentrations andas/particle partitioning of polycyclic aromatic hydrocarbonsopposite result for gas-phase PAHs. There were obviousin an urban site in Turkey. Ermvirormental Forensics, 7(4): 303-ifferences of total Pahs in different functional areaswhich has the highest concentration in industrial area Esen F, Tasdemir Y, Vardar N, 2008. Atmospheric concentrations of(LL) and commercial area(XY), followed by suburbanPAHs, their possible sources and partitioning at a residential(UE), and TX as background sampling sites has the lowestsite of Bursa, Turkey. Atmospheric Research, 88(3-4): 243-concentration of PAhsGaseous/particulate partitioning of PAHs showed moreFernandez p, grimalt J O, Vilanova R M, 2002. Atmospheric gas-particle partitioning of polycyclic aromatic hydrocarbons inshallow slopes(mr =-0.58)and steeper slope(mr-0.72)were observed in autumn and winter sampling time,V凵中国煤化工mmrespectively. The mr varied depending on specific charac- GalarCNMHG2006. Seasonality andteristics of sampling site and meteorological conditionsC-e partitioning of PAHThe correlation of the concentration for individual pahsobserved by the integrated atmospheric deposition networkfive sampling sites and diagnostic ratio analysis resultsADN). Atmospheric Evironment, 40(1): 182 -1Jinping Zhao et alGigliotti C L Dachs J, Nelson E D, Brunciak P A, Eisenreich S JTurpin B J et al., 2003. Gas/particle distribution of polycyclic2000. Polycyclic aromatic hydrocarbons in the New Jerseyaromatic hydrocarbons in coupled outdoor/indoor atmospherecoastal atmosphere. Emvironmental Science and TechnologyAtmospheric Environment, 37(5): 703-719Offenberg J H, Baker J E, 1999. Aerosol size distributions ofGoss K, Schwarzenbach R P, 1998. Gas/solid and gas/iquid par-polycyclic aromatic hydrocarbons in urban and over-watertitioning ofcompounds: Critical evaluation of themospheres. Envirormental Science and Technology, 33(19)33243331and Technology, 32(14 ): 2025-2032Offenberg J H, Baker JE, 2000. Aerosol size distributions ofelemen-Guo Z G, Sheng L F Feng J L, Fang M, 2003. Seasonal variationtal and organic carbon inof solvent extractable organic compounds in the aerosols inAtmospheric Emvironment, 34(10): 1509-1517Qingdao, China. Atmospheric Emvironment, 37(13): 1825- Pankow J F, Bidleman T F, 1992. Interdependence of the slopes1834and intercepts from log-log correlations of measured gasgustafson K E, Dickhut R M, 1997. Particle/gas concentrations andparticulate partitioning and vapor pressure-1. Theory anddistributions of PAHs in the atmosphere of southern Chesa-analysis of available data. Atmospheric Environment, 26(6):peake Bay. Emvironmental Science and Technology, 31(11071-1080.147Halsall C J, Coleman P J, Davis B J, Burnett V, Waterhouse KParkSS, Kim Y J, Kang CH, 2002. Atmospheric polycyclic aromat-ic hydrocarbons in Seoul, Korea. Atmospheric Environment,Jones P H et al., 1994. Polycyclic aromatic hydrocarbons in36(17):2917-2924U.K. urban air Emvironmental Science and Technology, 28(13): Pinto J P, Stevens RK, Willis RD, Kellogg R Mamane Y, NovakJet2380-2386Harrad S, Laurie L, 2005. Concentrations, sources and temporalal,1998. Czech air quality monitoring and receptor modelingtudy. Environmental Science and Technology, 32(7): 843-854trends in atmospheric polycyclic aromatic hydrocarbons in Pio C A, Alves C A, Duarte A C, 2001. Identification, abundance andmajor conurbation. Joumal of Environmental Monitoring, 7(7)rigin of atmospheric organic particulate matter in a Portugueserural area. Atmospheric Environment, 35(8): 1365-137Kavouras I G, Koutrakis P, Tsapakis E, Lagoudaki E, Stephanoue Rogge W F, Hildemann L M, Mazurek M A, Cass GR, Simoneit B RG, Von Baer D et al., 2001. Source apportionment of urbanT,1993. Sources of fine organic aerosol: 2. Non-catalyst andparticulate aliphatic and polynuclear aromatic hydrocarbonstalyst-equipped automobiles and heavy duty diesel trucks(PAHs) using multivariate methods. Emvironmental ScienceEnvironmental Science and Technology, 27(4): 636-651and Technology, 35(11): 2288-2294Simcik M F, Franz TP, Zhang HX, Eisenreich S J. 1998. Gas-particleKhalili NR. Scheff P A, Holsen TM. 1995. pah sourcepartitioning of PCBs and PAHs in the Chicago Urban and adjafor coke oven, diesel and gasoline engines, highway如cent coastal atmosphere: States of equilibrium. Emvironmentalwood combustion emission. Atmospheric ErmvironmeScience and Technology, 32(2): 251-257533-542.Simicik M F. Zhang H, Eisenreich S J, Franz TP. 1997. Urban con-Lammel G, Sehili A M, Bond T C. Feichter J. Grassl H. 2009tamination of the chicago/coastal lake Michigan atmosphere byGas/particle partitioning and global distribution of polycyclicPCBs and PAHs during AEOLOS. Environmental Science anaromatic hydrocarbons-A modelling approach. Chemosphere,Technology,31():2141-214776(1):98-106Sun P, Blanchard P, Brice K A, Hites R A, 2006. Trends in poly-Lee L C, Ho K F, Chan L Y, Zielinska B, Chow J C, 2001. Polycycliccyclic aromatic hydrocarbon concentrations in the great lakesaromatic hydrocarbons(PAHs) and carbonyl compounds in atmosphere. Environmental Science and Technology, 40(20)urban atmosphere of Hong Kong. Atmospheric Evironment62216227(34):59495960.Terzi E, Samara C, 2004. Gas/particle partitioning of polycyclic aro.LiJ, Zhang G, LiX D, Qi S H, Liu Q, Peng X Z, 2006.Sourcematic hydrocarbons in urban, adjacent coastal, and continentalseasonality of polycyclic aromatic hydrocarbons(PAHs)in abackground sites of westen Greece. Emvironmental Sciencesubtropical city, Guangzhou, South China. Science of the TotalTechnology.38(19:49734978Environment,355(1-3):145-155sapakis M, Stephanou E G, 2005. Polycyclic aromatic hydrocarbonsLiang C, Pankow J F, 1996. Gas/particle partitioning of organicin the atmosphere of the Eastem Mediterranean. Emvironmentalcompounds to environmental tobacco smoke: Partitiodn coe-Science and Technology, 39(17): 6584-6590ficient measurements by desorption and comparison to urban US EPA, 2003. 1999 National Emissions Imyrticulate material. Emvironmental Science and TechnologyWashington, DC. ftp: //ftp. epa. gov/Emislnventory/finalnei30(9):2800-280599ver3/haps/Lohmann R, Northcott G L, Jones K C, 2000. Assessing the contribu- Vardar N, Tasdemir Y, Odabasi M. Noll K E, 2004. Characterizationtion of diffuse domestic burning as a source of PCDD/Fs, PCBs,of atmospheric concentrations and partitioning of PAHs in thend PAHs to the U. K atmosphere. Environmental Science andChicago atmosphere Science of the Total Ermvirorment, 327(Technology,34(14:2892-28993)163-174Motelay-Massei A, Hamer T, Shoeib M, Diamond M, Sterm G, Vardar N, Esen F. Tasdemir Y 2008. Seasonal concentrations andRosenberg B, 2005. Using passive air samplers to assess urban-partitioning of PAHs in a suburban site of Bursa, Turkeyral trends for persistent organic pollutants and polycyclicEnvironmental Pollution, 155(2): 298-307aromatic hydrocarbons. 2. Seasonal trends for PAHs, PCBs, Ye C X, Wang X H, Yin H L, Yuan w M, Hong H S, 2006and organochlorine pesticides. Environmental Science andCharacteristics of PAHs in PMlO aerosols collected from differ.Technology,39(15):5763-5773.Naumova YY, Eisenreich S J, Turpin B J, Weisel C P, Morandi M1532-1538.T, Colome SDet al, 2002. Polycyclic aromatic hydrocarbons Yunker Min the indoor and outdoor air of three cities in the U中国煤化工 itchell H R, GoyettEnvironmental Science and Technology, 36(12): 2552-2559amova YY, Offenberg J H, Eisenreich S J, Meng Q, Polidori A,CN Gf PAH source and八):489-515
-
C4烯烃制丙烯催化剂 2020-09-15
-
煤基聚乙醇酸技术进展 2020-09-15
-
生物质能的应用工程 2020-09-15
-
我国甲醇工业现状 2020-09-15
-
JB/T 11699-2013 高处作业吊篮安装、拆卸、使用技术规程 2020-09-15
-
石油化工设备腐蚀与防护参考书十本免费下载,绝版珍藏 2020-09-15
-
四喷嘴水煤浆气化炉工业应用情况简介 2020-09-15
-
Lurgi和ICI低压甲醇合成工艺比较 2020-09-15
-
甲醇制芳烃研究进展 2020-09-15
-
精甲醇及MTO级甲醇精馏工艺技术进展 2020-09-15