research article origin and distribution of pahs in

Research ArticleOrigin and Distribution of PAHs in Ambient ParticulateSamples at High Mountain Region in Southern China

Peng-hui Li1 Yan Wang2 Yu-hua Li3 Hong-li Li3 and Xianliang Yi45

1School of Environmental Science and Safety Engineering Tianjin University of Technology Tianjin 300384 China2School of Environmental Science and Engineering Shandong University Jinan 250100 China3Shandong Environmental Monitoring Center Jinan 250101 China4The Swire Institute of Marine Science The University of Hong Kong Pokfulam Hong Kong5State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012 China

Correspondence should be addressed to Peng-hui Li lipenghui406163com and Yan Wang wysdueducn

Received 6 June 2014 Revised 21 November 2014 Accepted 21 November 2014

Academic Editor Hesham El-Askary

Copyright copy 2015 Peng-hui Li et al This is an open access article distributed under the Creative Commons Attribution Licensewhich permits unrestricted use distribution and reproduction in any medium provided the original work is properly cited

To understand the deposition and transport of PAHs in southern China a measurement campaign was conducted at a high-elevation site (the summit ofMount Heng 1269mASL) fromApril 4 toMay 31 2009 and a total of 39 total suspended particulatesamples were collected for measurement of PAH concentrations The observed particulate-bound PAHs concentrations rangedfrom 163 to 2983 ngm3 with a mean concentration of 603 ngm3 BbF FLA and PYR were the predominant compounds Goodcorrelations were found between individual PAHs and meteorological parameters such as atmospheric pressure relative humidityand ambient temperatureThe backward trajectory analysis suggested that particulate samples measured at theMount Heng regionwere predominantly associated with the air masses from southern China while the air masses transported over northern andnorthwesternChina had relative higher PAHs concentrations Based on the diagnostic ratios and factor analysis vehicular emissioncoal combustion industry emission and unburned fossil fuels were suggested to be the PAHs sources atMount Heng site Howeverthe reactivity and degradation of individual PAHs could influence the results of PAH source profiles which deserves furtherinvestigations in the future

1 Introduction

Polycyclic aromatic hydrocarbons (PAHs) are a group ofwidespread environmental contaminants originating fromboth natural (eg forest fires and volcanoes) and anthro-pogenic sources (eg incomplete combustion and pyrolysisof fossil fuels or organic materials) Between the two sourceshuman activities (ie anthropogenic sources) contribute themost to PAHs emissions This is particularly the case inurban area or industrial areas where the PAHs sources canbe entirely anthropogenic [1ndash4] PAHs are persistent andaccumulative in environment and they can cause carcino-genic and mutagenic effects to living things Thus thesecompounds have received more and more attention by envi-ronmental scientists for the last several decades The emis-sion abatement of PAHs has been listed on the agenda of

international convention processes such as the 1979 GenevaConvention on Long-Range Transboundary Air PollutionSince 1990 reduction of PAHs emission has been reportedin US and European countries In contrast to those devel-oped countries the PAH emissions in China have beencontinuously increasing due to the rapid industrializationand economic development [5ndash7] The total PAH emissionin China was estimated to be about 25300 tons in the yearof 2003 and the major sources were suggested to be domesticcoal combustion biofuel burning and industry emission [5]

Once released into the atmosphere PAHs can partitionbetween vapor and particle phases which is dependent ontemperature and vapor pressure of the chemicals [8 9] PAHswith high molecular weight (4ndash6 rings) tend to be associ-ated with particle phase while those with lower molecularweight (2-3 rings) are often concentrated in the vapor phase

Hindawi Publishing CorporationAdvances in MeteorologyVolume 2015 Article ID 245438 8 pageshttpdxdoiorg1011552015245438

2 Advances in Meteorology

2000

1500

1000

500

0

Topo

grap

hica

l hei

ght (

m)

Figure 1 Geographical location of Mount Heng (cited from [36])

[10] During the course of their transport PAHs could beremoved from the atmosphere due to precipitation andordry depositionThrough the grasshopper effect PAHs can betransported to very long ranges from their original sources[11]

Although a considerable number of studies have beenconducted onmeasurements of PAHs in urban environmentlittle work has been done in rural sites Remote mountainregions particularly with altitude in the free troposphereare the unique environments for the study of atmosphericpollution load over continental areas and the study at remotemountain regions can help to get full assessment of the roleof the atmosphere in the global distribution of PAHs [12 13]In this study atmospheric particulate samples were collectedat the summit of Mt Heng which is in the transition regionbetween the free troposphere and boundary layer and serveas a regionally representative site for studying the long-rangetransport of pollutants in Southern China The objectives ofthe present studywere (1) to gain a primary understanding onthe distribution of particulate-bound PAHs at Mt Heng and(2) to examine the possible sources and transport patterns ofPAHs in the region

2 Materials and Methods

21 Site Description and Sample Collection TheMount Hengis located in Hunan Province south China and it is betweentwo major polluted industrialurban areasmdashthe Pearl Riverand Yangtze River deltas There are two big cities Shanghaiand Guangzhou situated 900 km to the east and 400 km tothe south of the Mount Heng respectively The sampling sitewas located at a meteorological station (27∘181015840N 112∘421015840E)which was set up in the 1937 at the summit of Mount Heng(1269m ASL) (Figure 1)

The sampling period was carried out from April 4 toMay 31 2009 Total suspended particulate (TSP) sampleswere collected on glass fibre filters by a middle-volume air

sampler (KC-300 Qingdao Laoshan Electronic InstrumentCompany) daily (22 hours from 10 am to 8 am) Thesampler was operated at a flow rate of 225 Lmin and a totalof 39 TSP samples were collected Prior to sampling all theglass fibre filters were combusted at 450∘C in an oven for 6 hto volatilize any organic contaminants After sampling theglass fibre filters were wrapped in aluminum foils and frozenat minus20∘C and PAHs analysis was then conducted within twoweeks after sampling

22 Sample Preparation and Analysis The glass fibre filterswere extracted by Accelerated Solvent Extractor (DionexASE 300) with acetonen-hexane (1 1 vv) solvents and theelute was purified using silica gel columns and condensedto exactly 1mL with rotary evaporation and nitrogen streamtechnique PAHs were then determined using gas chro-matography coupled to mass spectrometry (Shimadzu 2010plus) The details of the extraction and analysis procedurewere described elsewhere [1] Fifteen individual PAHs weredetected in this study (Table 1)

23 Quality Control Deuterated perylene-d12 was spikedto all the samples to monitor procedural performance Themean recoveries based on surrogates in samples were 984 plusmn64

Field and method blanks were analyzed using the sameprocedure as particulate samples and all the PAHs concen-trations were corrected for blanks The control calibrationstandardsweremeasured regularly to ensure the performanceof instrument during sample analysis

3 Results and Discussion

31 Concentrations of PAHs in Particulate Samples Descrip-tive statistics for all valid observations of PAHs concentra-tions in particulate samples collected at Mount Heng aresummarized in Table 2 The concentrations of PAHs varied

Advances in Meteorology 3

Table 1The abbreviations for PAH compounds and their detectionlimits

PAHs Abbreviation Detection limit (ng)Acenaphthylene ACY 4Acenaphthene ACE 5Fluorene FLU 5Phenanthrene PHE 3Anthracene ANT 4Fluoranthene FLA 7Pyrene PYR 4Benz[a]anthracene BaA 2Chrysene CHR 7Benzo[b]fluoranthene BbF 3Benzo[k]fluoranthene BkF 4Benzo[a]pyrene BaP 4Dibenz[ah]anthracene DahA 6Benzo[ghi]perylene BghiP 4Indeno[123-cd]pyrene IcdP 5

from 163 to 2983 ngm3 with a mean concentration of603 ngm3 BbF was the predominant compound with amean concentration of 086 ngm3 contributing to 1426 ofthe total PAH concentration FLA PHE and PYR comprisedthe second tier of dominant compounds with mean concen-trations of 077 074 and 060 ngm3 respectively Similardistribution of individual PAHshas been reported in previousstudies in China For the research done by our group at theMount Tai (the highest mountain at northern China 1534mASL) BbF FLA and PYR were the most abundant PAHcompounds in PM

25samples accounting for 2355 1421

and 1039 of the total PAH concentration respectively [1]Wang et al [14] also suggested that BbF was the predominantcompound of PAHs in PM

10samples in Beijing In 2012

China Environmental Protection Agency has published thelatest ambient air quality standards in which the BaP dailyand annual concentration limits were set at 25 ngm3 and10 ngm3 respectively The BaP concentration found in thisstudy met the standard Together with BaP several otherPAHs compounds including BaA BbF BkF IcdP and DahAwere suggested as potential carcinogenic compounds by theInternational Agency for Research on Cancer (IARC) Thetotal concentration of these six compounds was 230 ngm3accounting for 3814 of the total PAHs

The observed PAHs concentrations at the Mount Hengare comparable with our previous studies done at the MountTai (fine particles 688 ngm3 Table 3) [1] When comparingwith other areas the PAHs concentrations at Mount Hengare much lower than the results reported in urban cities orareas in China including Beijing [14] Guangzhou [15] andNorthern Plain [16] In contrast the PAHs concentrationsat Mount Heng were higher than the observed concen-trations at Waliguan (a global standard observation site3810m ASL 208 ngm3) [17] high mountain regions ofEurope (007ndash110 ngm3 2240ndash2413m) [18] Mt BachelorObservatory (MBO lt6 ngm3 2763m) [19] Far East Asia

Table 2 Statistical description of PAH concentrations in particulatesamples at Mount Heng

Species PAHs concentrations (ngm3)Range Mean SD

ACY Nd-011 002 003ACE Nd-056 010 015FLU Nd-085 022 023PHE 017ndash283 074 071ANT Nd-041 012 012FLA 015ndash488 077 097PYR 013ndash362 060 072BaA 005ndash168 027 033CHR Nd-380 052 080BbF Nd-424 086 088BkF 011ndash125 036 030BaP 008ndash147 035 031IcdP Nd-180 039 039DahA Nd-053 007 011BghiP 021ndash260 064 051PAHs 163ndash2983 603 587

(032 ngm3) North Pacific Ocean (014 ngm3) and theArctic area (048 ngm3) [20]

32 Correlations of Particulate-Bound PAH Levels with Mete-orological Parameters The meteorological conditions areimportant factors that can affect the deposition levels ofpollutants [21ndash23] In the present study meteorologicalparameters including atmospheric pressure (press) relativehumidity (RH) and ambient temperature (119879) were measuredduring the sampling period The correlation coefficientsbetween these meteorological parameters and particulate-bound PAHs were analyzed (Table 4) Good correlation wasfound between atmospheric pressure and several individualPAHs including BkF BaP IcdP and BghiP suggesting thathigh atmospheric pressure enhanced the bound of thesecompounds to the particulate phase In the study of Tianet al [21] significant negative correlation was observedbetween particulate-bound PAHs and ambient temperaturesuggesting the temperature dependence for PAHs Someother studies also highlighted the important role of tempera-ture in PAHs partitioning between gas and particulate phase[24 25] However in this present study only five individualPAH compounds including ACY ACE BkF IcdP and BghiPpresented significant negative correlation with temperatureIn addition ACE and FLU had good positive relationshipswith RH indicating their RH dependence

33 Transport Pattern and Sources of Particulate-BoundPAHs In previous studies atmospheric samples always havehigher deposition concentrations when they came fromthe more polluted area [2 10] Back trajectory analysiswas conducted in this study to characterize the particulatedeposition character influenced by different source regions


Table 3 Comparison of particulate-bound PAH levels between Mount Heng and other studies

Sampling site Sample type Altitude (m ASL) sumPAHs PAHs concentrations (ngm3) ReferenceMount Heng China TSP 1269m sum15 603 This researchMount Tai China PM25 1534m sum15 688 [1]Waliguan China TSP 3810m sum14 208 [17]High Mountain Regions Europe TSP 2240mndash2413m sum20 007ndash110 [18]MBO US TSP 2763m sum14 lt4 [19]Far East Asia TSP NA sum15 032 [20]North Pacific Ocean TSP NA sum15 014 [20]Arctic TSP NA sum15 048 [20]Beijing China PM10 NA sum15 449 [14]Northern Plain China TSP NA sum16 346 [16]Guangzhou China TSP NA sum16 195 [15]

Table 4 The correlation coefficients between particulate bound-PAH concentrations and meteorological parameters

Press (Pa) 119879 (∘C) RH ()PAHs 0627 minus0639 0226ACY 0551 minus0764lowast 0665ACE minus0025 minus0234 0940lowastlowast

FLU minus0078 minus0166 0938lowastlowast

PHE 0389 minus0554 0700ANT 0472 minus0641 0621FLA 0541 minus0571 0119PYR 0555 minus0564 0076BaA 0572 minus0537 0050CHR 0531 minus0475 0015BbF 0688 minus0644 0174BkF 0733lowast minus0718lowast 0233BaP 0722lowast minus0706 0221IcdP 0767lowast minus0783lowast 0336DahA 0626 minus0656 0363BghiP 0751lowast minus0784lowast 0310Significance level lowast119875 lt 005 lowastlowast119875 lt 001

Forty-eight-hour backward trajectories were calculated usingthe HYSPLIT (hybrid single-particle Lagrangian integratedtrajectory) model at a height of 1269m ASL

Based on the analysis four major trajectory categorieswere classified for the samples NNW continental air massesfrom northern and northwestern China the most pollutedregion of China EA air masses from eastern China whereShanghai and its surrounding cities located here S airmassesfrom the Southern China transported through the PearlRiver Delta region and L samples with looped and shorttrajectories that stayed within a radius of 500 km of samplingsite (Figure 2)

Among the four classified trajectory categories S hap-pened most frequently accounting for 429 of the totalfollowed by NNW (371) EA (143) and L (57) Aspresented in Figure 3 the order of PAHs concentrationsamong the trajectory categories was NNW L EA and S

Longitude (∘E)

Latit

ude

(∘N

)

50

40

30

20

10

80 90 100 110 120 130 140

Figure 2 Classified pathway of each trajectory category

NNW S EA L0123456789

101112

57

143429

BghiPDahAIcdPBaPBkFBbFCHRBaA

PYRFLAANTPHEFLUACEACY

371

PAH

s con

cent

ratio

ns (n

gm

3)

Figure 3 PAHs concentrations based on different trajectory cate-gories


03 04 05 06

01

02

03

04

05

06Unburned petroleum Petroleum combustion Biomasscoal

Petro

leum

com

bust

ion

Unb

urne

d pe

trole

umBi

omas

sco

al

TSP

FLAFLA + PYR

IcdP

IcdP

+Bg

hiP

(a)

01 02 03 04 05 06 07

01

02

03

04

05Biomasscoal combustion

Petro

leum

Bi

omas

sco

al co

mbu

stio

n

Petroleum

TSP

BaABaA + CHR

AN

TA

NT+

PHE

(b)

Figure 4 Diagnostic PAH ratios for TSP samples collected at Mount Heng

The air masses of NNW group originated from the northernand northwestern China where most industrial activities ofChina are located and burning of coal and biomass was thedominant energy source So particulate samples of this grouphad the highest PAHs concentrations reaching 1071 ngm3Unexpectedly the group of L had higher PAHs concentra-tions than EA and S groups and the average concentrationreached 601 ngm3 PHE was the predominant compound ofL group contributing over 20 of the total concentrationAs presented in the study of Lin et al [26] PHE is a majorcomponent of emissions from incense burning There areseveral temples located in the Mount Heng region andmost of them are crowded with visitors Therefore incenseburning inside or outside the temples is suggested to be animportant local PAHs emission source It should be notedthat the relative fewer sample numbers of L group could causeuncertainties to some degree Air mass from eastern andsouthern China the two most developed areas in China hadlower PAHs concentrations which are 423 and 429 ngm3respectively

34 Diagnostic Ratios of PAH As suggested in prior studiesthe concentrations and ratios of some tracer PAHs couldbe used to identify the contribution of different sourcesFour common diagnostic ratios including FLA(PYR + FLA)IcdP(BghiP + IcdP) ANT(PHE + ANT) and BaA(BaA +CHR) were used to analyze the PAHs in particulate samplesand the results are presented in Figure 4

According to the study of Yunker et al [27] the ratioof FLA(PYR + FLA) lower than 04 implies the unburnedpetrogenic sources and the ratio higher than 05 signalsthe coal and wood combustion and a ratio between 04and 05 indicates the liquid fossil fuel combustion sourcesIn this study the ratio was 056 for particulate sampleindicating wood and coal combustion was the main source

For IcdP(BghiP + IcdP) the ratio lower than 02 suggestsunburned petrogenic sources the ratio between 02 and 04indicates liquid fossil fuel combustion sources and the ratiohigher than 05 signals the contribution of coal or woodcombustion [6] The ratio value was 038 for the sampleindicating comprehensive contributions from coal and liquidfossil fuel combustion sources For another common usedindicator ANT(PHE + ANT) a ratio lower than 01 signalsthe liquid fossil fuel sources and a ratio higher than 01indicates the combustion sources As presented in Figure 4the ratios were all above 01 for particulate samples indicatingthe combustion source contributions In previous study theratio of BaA(BaA +CHR) higher than 035 indicates the coalor other biomass combustion sources while the ratio lowerthan 02 signals the liquid fossil fuel sources [28] In this studythe ratio was 029 for particulate sample indicating the coaland liquid fossil fuel combustion contribution

Based on the results of diagnostic ratios analysis coalcombustion and emissions from liquid fossil fuel con-sumption were suggested to be the dominating sources ofparticulate-bound PAHs at Mount Heng site In our previousstudies conducted at Mount Tai the highest mountain innorthern China coal combustion and vehicular emissionswere the main sources of PAHs in atmospheric samplesas well [1 2] The results obtained from the high altitudebackground sites could reflect an overall picture of PAHpossible sources in China However special caution shouldbe given when using diagnostic ratios The ratio valuescould be altered as PAHs can react with other atmosphericcompounds such as hydroxyl radicals andor ozone [29 30]In addition degradation during the transport can modifythe concentrations and ratios of PAHs which is anotherlimitation of using diagnostic ratios [31] For example BaAand ANT have been proved to degrade more quickly thantheir isomers-CHR and PHE respectively [32 33]


Table 5 Factor analysis for particulate-bound PAHs

PAHs Factor 1 Factor 2ACY 0735ACE 0977FLU 0962PHE 0790ANT 0846FLA 0857PYR 0882BaA 0940CHR 0922BbF 0954BkF 0709BaP 0810IcdP 0851DahA 0895BghiP 0833 of variance 7077 1543

Sources Vehicular and coalcombustion emission

Unburned fossil fuelsand incense burning

35 Factor Analysis As stated above several constraints existwhen using diagnostic ratios to identify PAHs sources Factoranalysis which served as an exploratory tool can be used toquantify the major sources of PAHs In this present studythe total concentrations of 15 PAHs compounds detected inparticulate samples were subjected to factor analysis usingSPSS version 16 (SPSS Inc) Factor analysis was conductedwith Varimax rotation and factors with eigenvalue gt1 wereconsideredThe results of rotated factors are listed in Table 5

Two factors were separated accounting for 862 of thetotal variance in the data Factor 1 which explained 7077 ofthe variance presented high loading for individual PAHswithhigher molecular weight including FLA PYR BaA CHRBbF BkF BaP IcdP DahA and BghiP According to previousstudies BbF BkF IcdP and BghiP are the major componentsof vehicular emission and the presence of FLA PYR BaAand CHR could point to coal and wood combustion sources[1 34 35] Thus factor 1 could represent sources fromvehicular and coal combustion emission Factor 2 whichexplained 1543 of the variance is highly loaded on ACYACE FLU PHE and ANT ACY and ACE could signalthe contribution of unburned fossil fuels PHE and ANThave been identified in industry emission in previous studies[1 6] PHE is also a major component of emissions fromincense burning [26] while Flu could originate fromdifferentsources

Based on the results of factor analysis vehicular emissioncoal combustion industry emission and unburned fossilfuels were suggested to be the PAHs sources at MountHeng site However as mentioned earlier the reactivity anddegradation of individual PAHs could influence the resultsfor profiles of PAH sources and thus much work still needsto be conducted in the future

4 Conclusion

Particulate-bound PAHs concentrations were investigated athigh mountain region in Southern China from April toMay 2009 The PAH concentrations ranged from 163 to2983 ngm3 with a mean concentration of 603 ngm3 Themeteorological parameters including atmospheric pressurerelative humidity and ambient temperature had good cor-relations with individual PAHs The results obtained fromair mass back trajectories and PAHs concentrations high-lighted the importance of air mass origin The air masses ofNNW group transported over the most polluted region ofChina had relatively higher PAH concentrations Both thediagnostic ratio and factor analysis suggested that vehicularemission coal combustion industry emission and unburnedfossil fuels were the possible sources of PAHs at Mount Hengsite

Conflict of Interests

The authors declare that there is no conflict of interestsregarding the publication of this paper

Acknowledgments

The authors are grateful to Mount Heng MeteorologicalStation for providing meteorological data and other sup-port in the field observation They thank Jinan Institute ofEnvironmental Protection for the support of sample analysisThey appreciate the assistance from Zaifeng Wang HouyongZhang Likun Xue Xiaomei Gao Wei Nie and ShengzhenZhou This study was supported by the National NaturalScience Foundation of China (21177073 41475115) Tianjin 131creative talents project and Tianjin High School Science ampTechnology Fund Planning Project (20140515)

References

[1] P-H Li Y Wang Y-H Li et al ldquoCharacterization of polycyclicaromatic hydrocarbons deposition in PM25 and cloudfogwater at Mount Taishan (China)rdquo Atmospheric Environmentvol 44 no 16 pp 1996ndash2003 2010

[2] Y Wang P-H Li H-L Li X-H Liu and W-X Wang ldquoPAHsdistribution in precipitation at Mount Taishan China Identi-fication of sources and meteorological influencesrdquo AtmosphericResearch vol 95 no 1 pp 1ndash7 2010

[3] S S Park Y J Kim and C H Kang ldquoAtmospheric polycyclicaromatic hydrocarbons in Seoul Koreardquo Atmospheric Environ-ment vol 36 no 17 pp 2917ndash2924 2002

[4] C Vasilakos N Levi TMaggos J Hatzianestis JMichopoulosand C Helmis ldquoGas-particle concentration and characteriza-tion of sources of PAHs in the atmosphere of a suburban areain Athens Greecerdquo Journal of Hazardous Materials vol 140 no1-2 pp 45ndash51 2007

[5] S Xu W Liu and S Tao ldquoEmission of polycyclic aromatichydrocarbons in ChinardquoEnvironmental Science and Technologyvol 40 no 3 pp 702ndash708 2006

[6] K Ravindra R Sokhi and R van Grieken ldquoAtmosphericpolycyclic aromatic hydrocarbons source attribution emission


factors and regulationrdquo Atmospheric Environment vol 42 no13 pp 2895ndash2921 2008

[7] P-H Li S-F Kong C-M Geng et al ldquoHealth risk assessmentfor vehicle inspection workers exposed to airborne polycyclicaromatic hydrocarbons (PAHs) in their work placerdquo Environ-mental Sciences Processes and Impacts vol 15 no 3 pp 623ndash632 2013

[8] J He and R Balasubramanian ldquoSemi-volatile organic com-pounds (SVOCs) in ambient air and rainwater in a tropical envi-ronment concentrations and temporal and seasonal trendsrdquoChemosphere vol 78 no 6 pp 742ndash751 2010

[9] M F Simcik T P Franz H Zhang and S J EisenreichldquoGas-particle partitioning of PCBs and PAHs in the Chicagourban and adjacent coastal atmosphere states of equilibriumrdquoEnvironmental Science and Technology vol 32 no 2 pp 251ndash257 1998

[10] M A Olivella ldquoPolycyclic aromatic hydrocarbons in rainwaterand surface waters of Lake Maggiore a subalpine lake inNorthern Italyrdquo Chemosphere vol 63 no 1 pp 116ndash131 2006

[11] J He and R Balasubramanian ldquoA study of precipitation scav-enging of semivolatile organic compounds in a tropical areardquoJournal of Geophysical Research D Atmospheres vol 114 no 12Article ID D12201 2009

[12] G L Daly and FWania ldquoOrganic contaminants in mountainsrdquoEnvironmental Science and Technology vol 39 no 2 pp 385ndash398 2005

[13] B L van Drooge J O Grimalt C J Torres Garcıa andE Cuevas ldquoSemivolatile organochlorine compounds in thefree troposphere of the Northeastern Atlanticrdquo EnvironmentalScience and Technology vol 36 no 6 pp 1155ndash1161 2002

[14] WWang S LM SimonichWWang et al ldquoAtmospheric poly-cyclic aromatic hydrocarbon concentrations and gasparticlepartitioning at background rural village and urban sites in theNorth China Plainrdquo Atmospheric Research vol 99 no 2 pp197ndash206 2011

[15] Y Yang P Guo Q Zhang D Li L Zhao and D Mu ldquoSeasonalvariation sources and gasparticle partitioning of polycyclicaromatic hydrocarbons in Guangzhou Chinardquo Science of theTotal Environment vol 408 no 12 pp 2492ndash2500 2010

[16] S Liu S Tao W Liu et al ldquoAtmospheric polycyclic aromatichydrocarbons in north China a winter-time studyrdquo Environ-mental Science and Technology vol 41 no 24 pp 8256ndash82612007

[17] H-R Cheng G Zhang X Liu J Li S-H Qi and Y-C ZhaoldquoStudies on polycyclic aromatic hydrocarbons in the atmo-sphere ofWaliguanQinghairdquoChina Environmental Science vol26 no 6 pp 646ndash649 2006

[18] P Fernandez J O Grimalt and R M Vilanova ldquoAtmosphericgas-particle partitioning of polycyclic aromatic hydrocarbonsin high mountain regions of Europerdquo Environmental Science ampTechnology vol 36 no 6 pp 1162ndash1168 2002

[19] T Primbs A Piekarz G Wilson et al ldquoInfluence of Asian andWestern United States urban areas and fires on the atmospherictransport of polycyclic aromatic hydrocarbons polychlorinatedbiphenyls and fluorotelomer alcohols in the Western UnitedStatesrdquo Environmental Science and Technology vol 42 no 17pp 6385ndash6391 2008

[20] X Ding X M Wang Z Q Xie et al ldquoAtmospheric polycyclicaromatic hydrocarbons observed over the North Pacific Oceanand the Arctic area Spatial distribution and source identifica-tionrdquo Atmospheric Environment vol 41 no 10 pp 2061ndash20722007

[21] F Tian J Chen X Qiao et al ldquoSources and seasonal variationof atmospheric polycyclic aromatic hydrocarbons in DalianChina factor analysis with non-negative constraints combinedwith local source fingerprintsrdquo Atmospheric Environment vol43 no 17 pp 2747ndash2753 2009

[22] K Ravindra L Bencs E Wauters et al ldquoSeasonal and site-specific variation in vapour and aerosol phase PAHs over Flan-ders (Belgium) and their relationwith anthropogenic activitiesrdquoAtmospheric Environment vol 40 no 4 pp 771ndash785 2006

[23] A Motelay-Massei D Ollivon B Garban and M ChevreuilldquoPolycyclic aromatic hydrocarbons in bulk deposition at asuburban site assessment by principal component analysisof the influence of meteorological parametersrdquo AtmosphericEnvironment vol 37 no 22 pp 3135ndash3146 2003

[24] M Tsapakis and E G Stephanou ldquoOccurrence of gaseousand particulate polycyclic aromatic hydrocarbons in the urbanatmosphere study of sources and ambient temperature effect onthe gasparticle concentration and distributionrdquo EnvironmentalPollution vol 133 no 1 pp 147ndash156 2005

[25] A Li J-K Jang and P A Scheff ldquoApplication of EPA CMB82model for source apportionment of sediment PAHS in LakeCalumet Chicagordquo Environmental Science and Technology vol37 no 13 pp 2958ndash2965 2003

[26] T-C Lin F-H Chang J-H Hsieh H-R Chao and M-RChao ldquoCharacteristics of polycyclic aromatic hydrocarbons andtotal suspended particulate in indoor and outdoor atmosphereof a Taiwanese templerdquo Journal of Hazardous Materials vol 95no 1-2 pp 1ndash12 2002

[27] M B Yunker R W Macdonald R Vingarzan R H MitchellD Goyette and S Sylvestre ldquoPAHs in the Fraser River basin acritical appraisal of PAH ratios as indicators of PAH source andcompositionrdquoOrganic Geochemistry vol 33 no 4 pp 489ndash5152002

[28] H H Soclo P Garrigues and M Ewald ldquoOrigin of polycyclicaromatic hydrocarbons (PAHs) in coastal marine sedimentscase studies in Cotonou (Benin) and Aquitaine (France) AreasrdquoMarine Pollution Bulletin vol 40 no 5 pp 387ndash396 2000

[29] A L Robinson R Subramanian N M Donahue A Bernardo-Bricker and W F Rogge ldquoSource apportionment of molecularmarkers and organic aerosolmdash1 Polycyclic aromatic hydrocar-bons and methodology for data visualizationrdquo EnvironmentalScience and Technology vol 40 no 24 pp 7803ndash7810 2006

[30] A L Robinson N M Donahue andW F Rogge ldquoPhotochem-ical oxidation and changes inmolecular composition of organicaerosol in the regional contextrdquo Journal of Geophysical ResearchD Atmospheres vol 111 no 3 Article ID D03302 2006

[31] M Tsapakis and E G Stephanou ldquoCollection of gas and particlesemi-volatile organic compounds use of an oxidant denuderto minimize polycyclic aromatic hydrocarbons degradationduring high-volume air samplingrdquo Atmospheric Environmentvol 37 no 35 pp 4935ndash4944 2003

[32] R M Kamens Z Guo J N Fulcher and D A Bell ldquoInfluenceof humidity sunlight and temperature on the daytime decayof polyaromatic hydrocarbons on atmospheric soot particlesrdquoEnvironmental Science and Technology vol 22 no 1 pp 103ndash108 1988

[33] J J Schauer W F Rogge L M Hildemann M A MazurekG R Cass and B R T Simoneit ldquoSource apportionmentof airborne particulate matter using organic compounds astracersrdquo Atmospheric Environment vol 30 no 22 pp 3837ndash3855 1996


[34] H Guo S C Lee K F Ho XMWang and S C Zou ldquoParticle-associated polycyclic aromatic hydrocarbons in urban air ofHongKongrdquoAtmospheric Environment vol 37 no 38 pp 5307ndash5317 2003

[35] WZhang S Zhang CWanD Yue Y Ye andXWang ldquoSourcediagnostics of polycyclic aromatic hydrocarbons in urban roadrunoff dust rain and canopy throughfallrdquo Environmental Pol-lution vol 153 no 3 pp 594ndash601 2008

[36] J Zhou YWang T X Yue YH Li K-MWai andWXWangldquoOrigin and distribution of trace elements in high-elevationprecipitation in Southern Chinardquo Environmental Science andPollution Research vol 19 no 8 pp 3389ndash3399 2012

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2000

1500

1000

500

0

Topo

grap

hica

l hei

ght (

m)

Figure 1 Geographical location of Mount Heng (cited from [36])

[10] During the course of their transport PAHs could beremoved from the atmosphere due to precipitation andordry depositionThrough the grasshopper effect PAHs can betransported to very long ranges from their original sources[11]

Although a considerable number of studies have beenconducted onmeasurements of PAHs in urban environmentlittle work has been done in rural sites Remote mountainregions particularly with altitude in the free troposphereare the unique environments for the study of atmosphericpollution load over continental areas and the study at remotemountain regions can help to get full assessment of the roleof the atmosphere in the global distribution of PAHs [12 13]In this study atmospheric particulate samples were collectedat the summit of Mt Heng which is in the transition regionbetween the free troposphere and boundary layer and serveas a regionally representative site for studying the long-rangetransport of pollutants in Southern China The objectives ofthe present studywere (1) to gain a primary understanding onthe distribution of particulate-bound PAHs at Mt Heng and(2) to examine the possible sources and transport patterns ofPAHs in the region

2 Materials and Methods

21 Site Description and Sample Collection TheMount Hengis located in Hunan Province south China and it is betweentwo major polluted industrialurban areasmdashthe Pearl Riverand Yangtze River deltas There are two big cities Shanghaiand Guangzhou situated 900 km to the east and 400 km tothe south of the Mount Heng respectively The sampling sitewas located at a meteorological station (27∘181015840N 112∘421015840E)which was set up in the 1937 at the summit of Mount Heng(1269m ASL) (Figure 1)

The sampling period was carried out from April 4 toMay 31 2009 Total suspended particulate (TSP) sampleswere collected on glass fibre filters by a middle-volume air

sampler (KC-300 Qingdao Laoshan Electronic InstrumentCompany) daily (22 hours from 10 am to 8 am) Thesampler was operated at a flow rate of 225 Lmin and a totalof 39 TSP samples were collected Prior to sampling all theglass fibre filters were combusted at 450∘C in an oven for 6 hto volatilize any organic contaminants After sampling theglass fibre filters were wrapped in aluminum foils and frozenat minus20∘C and PAHs analysis was then conducted within twoweeks after sampling

22 Sample Preparation and Analysis The glass fibre filterswere extracted by Accelerated Solvent Extractor (DionexASE 300) with acetonen-hexane (1 1 vv) solvents and theelute was purified using silica gel columns and condensedto exactly 1mL with rotary evaporation and nitrogen streamtechnique PAHs were then determined using gas chro-matography coupled to mass spectrometry (Shimadzu 2010plus) The details of the extraction and analysis procedurewere described elsewhere [1] Fifteen individual PAHs weredetected in this study (Table 1)

23 Quality Control Deuterated perylene-d12 was spikedto all the samples to monitor procedural performance Themean recoveries based on surrogates in samples were 984 plusmn64

Field and method blanks were analyzed using the sameprocedure as particulate samples and all the PAHs concen-trations were corrected for blanks The control calibrationstandardsweremeasured regularly to ensure the performanceof instrument during sample analysis

3 Results and Discussion

31 Concentrations of PAHs in Particulate Samples Descrip-tive statistics for all valid observations of PAHs concentra-tions in particulate samples collected at Mount Heng aresummarized in Table 2 The concentrations of PAHs varied


























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4 Conclusion




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Volume 2014

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4 Conclusion




Acknowledgments


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Volume 2014

Mining


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Geology Advances in











































Volume 2014

Mining


Journal of



Geophysics







Journal of




Advances in











Geology Advances in

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