17Contamination of sealed urban soils with PAHs

http://www.degruyter.com/view/j/ssa (Read content)

SOIL SCIENCE ANNUALVol. 67 No. 1/2016: 17–23

* Dr. P. Charzyñski, pecha@umk.pl

DOI: 10.1515/ssa-2016-0003

DE DE GRUYTER

OPEN

INTRODUCTION

Polycyclic aromatic hydrocarbons (PAHs) areorganic compounds composed of two or more fusedaromatic benzene rings as part of their structure. Theycan arrive into the environment components, like soils,from both natural, anthropogenic, and technogenicsources (Tsibart and Gennadiev 2012). PAHs belongto a group of persistent organic pollutants (Vacha etal. 2010) due to their chemically stable structure andlow bioavailability (Lamichhane et al. 2016). Despitethe fact that there is a large amount of research on thecontamination of different landscape components(including soils), many problems related to the originand behavior of PAHs in the environment are stillunclear (Tsibart and Gennadiev 2012).

Soil sealing has a significant impact on the func-tioning of soil. This problem often affects fertile agri-cultural lands, increases the flood risk and waterdeficiency, and contributes to global warming(Couch et al. 2007, Scalenghe and Ajmone Marsan2009, EU Technical Report 2011). Sealing of soils islisted as one of the main causes of soil degradation inthe European Union together with soil erosion,decrease of soil organic matter content, soil compaction,etc. (European Commission 2006). There are twoexamples of the degree of soil sealing (Nestroy 2006).

First of them is the total imperviousness (caused bysolid concrete or asphalt), the second is sealing withsemi-pervious surface (e.g. cobblestones, concretepaving slabs or openwork concrete structures) whichallow partial penetration of water and air.

The objective of the study was to determine theinfluence of soil sealing degree on soil contaminationwith polycyclic aromatic hydrocarbons (PAHs).

MATERIAL AND METHODS

The study area included four (A, B, C, D) samplingsites located within the administrative boundaries ofthe Toruñ city, Poland (Fig. 1). Detailed characteri-zation of each sampling site is presented in Table 1.

Sampling procedure involved preparation of soilpits representing three examples of soil sealing at eachsite. These examples are: non-sealed soil as a controlone (I) and two degrees of soil sealing: semi-pervioussurface (II) and totally impervious surface (III). Atsampling site “A” only the control profile (I) and theprofile sealed with the semi-pervious surface (II) havebeen studied. Field works were conducted betweenApril of 2012 and September of 2013.

Samples from sealed soil were collected fromtopmost horizon (top 10 cm of it, if thicker) thatsurvived the process of pavement construction and

£UKASZ MENDYK, PRZEMYS£AW CHARZYÑSKI*

Nicolaus Copernicus University in Toruñ, Faculty of Earth SciencesDepartment of Soil Science and Landscape Management, Lwowska St. 1, 87-100 Toruñ, Poland

Soil sealing degree as factor influencing urban soil contaminationwith polycyclic aromatic hydrocarbons (PAHs)

Abstract: The objective of the study was to determine role of soil sealing degree as the factor influencing soil contamination withpolycyclic aromatic hydrocarbons (PAHs). The study area included four sampling sites located within the administrative boundariesof the Toruñ city, Poland. Sampling procedure involved preparing soil pits representing three examples of soil sealing at each site:non-sealed soil as a control one (I) and two degrees of soil sealing: semi-pervious surface (II) and totally impervious surface (III).Together with basic properties defined with standard procedures (particle size distribution, pH, LOI, content of carbonates) contentof selected PAHs was determined by dichloromethane extraction using gas chromatography with mass spectrometric detection (GC-MS). Obtained results show that urban soils in the city of Toruñ are contaminated with polycyclic aromatic hydrocarbons. Soilsealing degree has a strong influence on the soil contamination with polycyclic aromatic hydrocarbons. Totally sealed soils are betterpreserved from atmospheric pollution including PAHs. Combustion of grass/wood/coal was the main source of determined PAHscontent in examined soils.

Keywords: technogenic soils, urban soils, Ekranic Technosols, soil sealing, soil contamination, PAHs

18 £UKASZ MENDYK, PRZEMYS£AW CHARZYÑSKI

from the corresponding horizons in case of non-sealedsoils. Detailed sampling depths were described inTable 1. In total, 11 samples were collected for thelaboratory analysis. The following soil properties weredetermined: particle size distribution by the sievemethod and the hydrometer method (the Bouyoucosaerometric method modified by Cassagrande and Pró-szyñski), the names of the texture classes were givenin line with the classification of Soil Science Societyof Poland – PTG 2008 (Polskie Towarzystwo Gle-boznawcze 2009), pH potentiometrically for the soil-to-solution ratio of 1:2.5 using H2O and 1 mol·dm3

KCl as the suspension medium, approximate contentof organic matter was determined using loss on igni-

tion (LOI) analysis (each sample was ignited attemperatures of 550° in a muffle furnace), and contentof carbonates by the Scheibler volumetric method.Content of selected PAHs was determined by dichlo-romethane extraction using gas chromatography withmass spectrometric detection (GC-MS) according tothe US GEOLOGICAL SURVEY procedure (Furlonget al.1996) with following detection limits and meanmethod recovery (compound – detection limit/methodrecovery, both in µg·kg–1): acenaphthylene – 0.2/1.02,acenaphthene – 0.3/0.63, fluorene – 0.3/0.83,phenanthrene – 0.2/0.99, anthracene – 0.3/0.91,fluoranthene – 0.3/0.97, pyrene – 0.3/0.90,benzo[a]anthracene – 0.3/1.04, chrysene – 0.2/1.01,

FIGURE 1. Location of the study area

TABLE 1. Sampling sites and soil profile descriptions

eliforP.oN

gnilpmaShtped

)noitaziretcarahcetis;teerts;noitcesyticevitartsinimda(noitpircsedetiS

IA 12–21 ;noitcesyticynaleiBteerts–teertSakceineimezrKehtta

supmaCUCNehtfotrapagnieb

IIAeliforproflortnoc:ssarghtiwderevoctlebneergedisdaor

IIA 12–21 m57.0x1dezissbalsetercnochtiwdelaesedisdaorehtselohmc01x5htiw

IB 42–41 aeradetserof–ezcêjaZyróGstocShtiwylniamderevocsenuddnas(

ehtdnaynaleiBehtneewteb)senip;snoitcesyticeicœeimdezrPeiksñim³ehC

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IIB 71–11 )"kurblop"dellacos(stesetercnocllamshtiwdelaesklawedis

IIIB 71–11 tnemevapsuonimutibhtiwdelaesyawklaw

IC 91–9 ;noitcesyticeiprakSaNtrapnretsae–teertSakcibuLehtta

nretsaeehtfoerafhguorohtrojamehtfoyticehtfotrap

IIICdnaIICseliforproflortnoc:ssarghtiwderevoctlebneergedisdaor

IIC 71–7 3.0x3.0dezissbalsetercnocdiloshtiwdelaesyawklaw

IIIC 81–8 tnemevapsuonimutibhtiwdelaesyawklaw

ID 73–72 ;noitcesyticzrógdoPotesolcteerts–teertSawopetSehttanrehtuosehtfoerafhguorohtrojameht

yticehtfotrap

IIIDdnaIIDeliforproflortnoc;tolpssarg

IID 73–72 ,mc01x5selohhtiwm1x1sbalsetercnochtiwdelaes;teertsssecca

IIID 73–72 sbalsetercnocdiloshtiwdelaes;teertsssecca

19Contamination of sealed urban soils with PAHs

benzo[b]fluoranthene – 0.5/1.04, benzo[k]fluoranthene– 0.3/1.10, benzo[e]pyrene – 0.3/0.97, benzo[a]pyrene– 0.4/0.97, perylene – 0.5/0.97, indeno[1,2,3-cd]pyrene– 0.3/1.20, dibenz[a,h]anthracene – 0.8/1.27, ben-zo[ghi]perylene – 1.0/1.20.

Box-and-whisker plots, (Fig. 2) were drawn usingStatistica 9.0 software (Statsoft Inc.) to show therelationships between some soil parameters and soilsealing degree.

RESULTS AND DISCUSSION

Basic properties of the soils studied

In general all of the analysed samples werecharacterized by the sandy texture (sandy loam in caseof sample B I) (Table 2). Therefore, the sealed soil

profiles (A II, B II, B III, C II, C III) meet the criteriaof Ekranic Technosols (Arenic) according to WRB(IUSS Working Group WRB 2015). According to thePolish Soil Classification (PSC 2011) they wereclassified as Ekranosols (in Polish: ekranosole).Reference soil profiles (A I, B I, C I, D I) arecharacterized by morphology features of deformed(truncated or buried with relocated material) BrunicArenosols (Rusty soils – gleby rdzawe; PSC 2011) orweakly developed Podzols (Podzolic soils – glebybielicowe; PSC) which dominated in the area of riverterraces in place when the city is located (Bednarekand Jankowski 2006, Charzyñski et al. 2013a).

Approximate content of soil organic mattermeasured based on LOI varied from 0.28 to 6.63%(Table 2) with no significant trend according to thesoil sealing degree. This result is in opposite to other

FIGURE 2. The differences in some ofthe investigated soil propertiesdepending on the soil sealing degree

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36.655.4

2.79.6

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8.77.75.7

8.65.42.6

4.43.77.5

9999001

110

000

dnas.mdnas.m.gdnas.m.g

IDIIDIIID

73–7273–7273–72

82.085.064.0

6.84.84.8

4.83.83.8

84.99.11

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TABLE 2. Selected physical and chemical properties of the investigated samples

* Textural class: m. – medium, c. – coarse, g. – gravelly, s. – sandy.

20 £UKASZ MENDYK, PRZEMYS£AW CHARZYÑSKI

reported findings that soil sealing has strong influenceon the organic carbon concentration (e.g. Pouyat etal. 2006, Churkina et al. 2010), as well as example ofdifferent studies from the Toruñ city concerning theimpact of soil sealing degree on microbial biomassand enzymatic activity (Charzyñski et al. 2013b,Piotrowska-D³ugosz and Charzyñski 2015). Thereaction of soils was alkaline in all analyzed samples.Differentiation of the pH values, as well as the CaCO3content was not connected with the soil sealing as incase of the organic matter content (LOI) (Table 2,Fig. 2).

PAHs content in studied soils, its variabilityand origin

PAHs content in analyzed soils was characterizedby large variability. It ranged from 73 to 5907 µg⋅kg–1

for the sum of the determined PAHs (Table 3). Eightout of nine compounds (beside the naphthalene) fromthe list defined in the Regulation the Polish Ministerof Environment (Regulation of the Minister of Envi-ronment 2002) were examined in this study. Definedlimits were exceeded for 46 individual cases and for5 out of 11 total samples in case of calculated sum ofthe listed PAHs for the depth of 0–0.3 m in the built-upand urban areas. Content of benzo[a]pyrene exceededthe allowable limits to the utmost, even more than 15times more in case of sample B I (Table 3).

Sum of the determined PAHs and benzo[a]pyrenecontent shows a significant impact of the soil sealingdegree on the soil contamination with polycyclicaromatic hydrocarbons (Fig. 2). Concentration of theseharmful compounds clearly decrease with the soilsealing degree as the totally sealed soils were the least,and non-sealed control ones were the most contami-nated. Therefore, despite the fact that soil sealing iswithout any doubt negative phenomenon some positiveimpact could be also present. In these case it is the sup-pressing of the atmosphere originated pollution. Thepositive aspect of some soil degrading factors e.g. soilerosion leading to the preservation of the organic soilswith the colluvium was reported already (e.g. Smól-czyñski 2006, Mendyk et al. 2015).

Fluoranthene and pyrene are dominating compoundswhen taking into accounts the means of the resultsobtained for all of the analyzed samples (Table 3).Similar results were obtained for the urban soils ofLondon (Vane et al. 2014). In case of some particularinstances this situation could be different. Theseexamples were samples characterized by dominationof benzo[b]fluoranthene and benzo[ghi]perylene incase of A II sample and indeno[1,2,3-cd]pyrene andbenzo[ghi]perylene for B I, respectively. All of thesefive compounds are listed as the pyrolytic compounds

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21Contamination of sealed urban soils with PAHs

coming from incomplete combustion of the oil andits products (Tsibart and Gennadiev 2012) or thecombustion of fossil fuels in general (McCready etal. 2000, Vane et al. 2007, Vane et al. 2014).

PAH isometric ratios were also used in order tocharacterize the PAH main source in soil and sediments(Vane et al. 2013, 2014). Following ratios were usedin these paper: phenathrene/anthracene comparedwith fluoranthene/pyrene (Budziñski et al. 1997, Vaneet al. 2014) and benzo[a]anthracene/benzo[a]anthra-

cene+chrysene compared with fluoranthene/fluoran-thene+pyrene (Yunker et al. 2002, Vane et al. 2014)(Fig. 3 and 4). Values of the first two ratios showsthat almost all of the samples were contaminated withPAH coming from pyrogenic sources (Fig. 3). This isconfirmed with results of another two ratios (Fig. 4)that suggest the combustion of grass/wood/coal as themain origin of PAHs in the soils studied. On the otherhand we can not exclude an illegal combustion ofsynthetic materials wastes e.g. plastic bottles as theother source of PAHs. Relatively high concentrationof benzo[ghi]perylene compared to benzo[a]pyrene(values exceeding 3.14) (Vane et al. 2014, afterCreaser et al. 2007) indicates the traffic exhaust asthe major source of pyrolytic source. The values ofthis ratio ranged from 0.81 to 1.67, therefore it standtogether with previous analyzed plots. All of the resultsare similar to those coming from the research conductedfor the city of London (Vane et al. 2014), Miami (Ban-ger et al. 2010), and New York (Marquez-Bravo et al.2016). However this method alone is not definitiveand could be a source of uncertainty (Vane et al. 2014after Katsoyiannis et al. 2007, 2011).

There are significant differences in PAHs concen-tration between individual study sites in Toruñ city.The highest content of analyzed compounds wasobserved on the Stepowa street (site D), in thesouthern part of the city. This site is also characterizedby the smallest variation in PAHs content accordingto the soil sealing degree. Relatively high concentrationswere also determined in samples collected at the sitesA and B. These three sites (A, B, and D) were distin-guished by location within or in the close vicinity tothe single-family residences, whereas the site C(Table 3) was located in the largest block of flathousing area in the city. This fact, together withresults explaining the grass/wood/coal combustion asthe main source of PAHs in soils examined suggestthat the individual heating systems of single-familyresidences are the main origin of these compounds instudied sites. The atmospheric source of the PAHs isobvious when analyzing the content of benzo[a]-pyrene in the air suspended particles at kujawsko-pomorska zone and for the city of Toruñ that in theperiod of 2009–2013 (WIOŒ Bydgoszcz 2014).

CONLCUSIONS

1. Urban soils in the city of Toruñ were contaminatedwith PAHs. Determined concentrations exceededthe defined limits for the surface soil horizons ofthe urban areas (Regulation of the Polish Ministerof Environment 2002), especially for the highlyharmful benzo[a]pyrene.

FIGURE 3. Isometric ratio plot of Phenathrene/Anthracene andFluoranthene/Pyrene

FIGURE 4. Isometric ratio plot of Benzo[a]anthracene/Benzo[a]anthracene+Chrysene and Fluoranthene/Fluoranthene+Pyrene

22 £UKASZ MENDYK, PRZEMYS£AW CHARZYÑSKI

2. Soil sealing degree has a strong influence on thesoil contamination with polycyclic aromatichydrocarbons. Totally sealed soils are preservedfrom atmospheric pollution including PAHs.

3. The main source of determined PAHs content inexamined soils was the combustion of grass/wood/coal, most probably coming from the individualheating systems of the single-family residences.

ACKNOWLEDGMENTS

Research was financed by the Polish Ministry ofScience and Higher Education (project No. N N306463738).

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Received: April 2, 2016Accepted: May 24, 2016

Stopieñ przykrycia gleby jako czynnik wp³ywaj¹cy na zanieczyszczeniegleb miejskich wielopierœcieniowymi wêglowodorami aromatycznymi (WWA)

Streszczenie: Celem badañ by³o okreœlenie roli stopnia zasklepienia gleb jako czynnika wp³ywaj¹cego na ich zanieczyszczeniewielopierœcieniowymi wêglowodorami aromatycznymi (WWA). Obszar badañ obejmowa³ cztery lokalizacje poboru próbek w obrê-bie granic administracyjnych miasta Torunia. Próbki zosta³y pobrane z profili glebowych reprezentuj¹cych trzy przyk³ady przykryciagleb: glebê nieprzykryt¹ jako profil kontrolny (I) oraz dwa stopnie zasklepienia gleb: powierzchni¹ czêœciowo przepuszczaln¹ (II)i nieprzepuszczaln¹ (III). Oprócz podstawowych w³aœciwoœci oznaczonych za pomoc¹ standardowych procedur (uziarnienie, pH,straty pra¿enia, zawartoœæ wêglanów) zosta³a oznaczona zawartoœæ wybranych WWA po ekstrakcji dichlorometanem za pomoc¹metody chromatografii gazowej z detekcj¹ spektrometri¹ mas. Uzyskane wyniki pozwalaj¹ stwierdziæ, ¿e gleby miejskie Torunia s¹zanieczyszczone WWA. Stopieñ zasklepienia gleb ma silny wp³yw na poziom tego zanieczyszczenia. Gleby ca³kowicie przykryte s¹lepiej chronione przed zanieczyszczeniami pochodzenia atmosferycznego, w tym wielopierœcieniowymi wêglowodorami aromatycz-nymi. Spalanie trawy/drewna/wêgla zosta³o zdiagnozowane jako g³ówne Ÿród³o oznaczonych zawartoœci WWA w badanych glebach.

S³owa kluczowe: gleby technogeniczne, gleby miejskie, Ekranic Technosols, zasklepianie gleb, zanieczyszczenie gleb, WWA