ENVIRONMENTAL

POLLUTION

Environmental Pollution 105 (1999) 67±74

Polycyclic aromatic hydrocarbons in Estonian soil: contamination

and pro®les
M. Trapido*
Department of Environmental Chemistry and Technology, Institute of Chemistry at Tallinn Technical University; 15, Akadeemia tee,
12618, Tallinn, Estonia

Received 27 April 1998; accepted 12 November 1998

Abstract
The distribution and accumulation of polycyclic aromatic hydrocarbons (PAH) in soil as well as PAH pro®les have been inves-
tigated in areas with di€erent anthropogenic pollution such as the city of Tallinn, the towns of PaÈrnu and Kohtla-JaÈrve and some
rural areas. PAH were identi®ed in 147 soil samples (0±10 cm upper layer) collected in September 1996. The typical  PAH level in
Estonian rural soil is about 100 mg/kg dry weight. PAH concentrations in Tallinn, PaÈrnu and Kohtla-JaÈrve soil were quite high (the
mean  PAH concentrations were 2240, 7665 and 12 390 mg/kg dry weight, respectively). The dominant PAH in soil samples were
pyrene, triphenylene and ¯uoranthene. 3±4 ring PAH and 5±6 ring PAH ratio altered from 5:1 to 1.7:1. # 1999 Elsevier Science
Ltd. All rights reserved.
Keywords: Polycyclic aromatic hydrocarbons (PAH); Contamination; Pro®les; Soil; Estonia

1. Introduction compound, from 2 month to 2 years (Mackay et al.,

Polycyclic aromatic hydrocarbons (PAH) released
into the environment arise mainly from anthropogenic
sources. They are mainly formed as by-products of
incomplete combustion of organic materials. PAH have
been identi®ed in many emission sources, such as vehicle
exhausts, power plants, chemical-, coke- and oil-shale
industries, urban sewage. Primary natural sources of
PAH are forest ®res and volcanic activity (Suess, 1976;
Shabad and Ilnitskii, 1979). United States Environ-
mental Protection Agency (US EPA) has identi®ed 16
PAHs as `priority pollutants'. PAH are important
environmentally because many individual PAH are
genotoxic (White et al., 1998) and may cause mutations
and certain types of cancer. PAH compounds convert
into carcinogens through metabolic activation in the
organism. In many circumstances the environmental
occurrence of PAH has been associated with adverse
e€ects on public health (Yang et al., 1991).
PAH are quite resistant to degradation. The range
of half-lives for PAH in soil estimated by di€erent
researchers is quite large. They vary, dependent on the
* Tel.: +372-2536-269; e-mail: trapido@chemnet.ee.
1992) and from 8 to 28 years (Wild et al., 1990). When
the release of PAH into the environment exceeds their
degradation capacity, a signi®cant accumulation of
PAH is observed. The existence of permanent pollution
sources results in the accumulation of PAH in soil,
plants and water bodies.
Soil contamination originates mainly from PAH
emissions to the atmosphere, which reach the soil via
precipitation. Gaseous and particle-bound PAH can be
transported over long distances before deposition
(Wania and Mackay, 1996). PAH are accumulated
mainly in the humus layer of soil. The further path-
ways of PAH dissipation in contaminated soil may be
volatilisation, irreversible sorption, leaching, accumu-
lation by plants, and biodegradation (Reilley et al.,
1996). PAH with three and more rings tend to be
strongly adsorbed to the soil. Strong sorption coupled
with very low water solubility and very low vapour
pressures make leaching and volatilisation insigni®cant
pathway of PAH dissipation (Park et al., 1990). Also
plants hardly take up any PAH from soil (Shabad and
Ilnitskii, 1979; Sims and Overcash, 1983). Soil bacteria
are the primary degraders of PAH in soil (Shabad and
Ilnitskii, 1979, Gibson and Subramanian, 1984; Boldrin
et al., 1993).

0269-7491/99/$Ðsee front matter # 1999 Elsevier Science Ltd. All rights reserved.
PII: S0269 -7 491(98)00207 -3
68 M. Trapido / Environmental Pollution 105 (1999) 67±74
PAH concentration in soil correlates signi®cantly
with the corresponding levels in air (Vogt et al., 1987),
house dust (Chuang et al., 1995), urban street dust
(Takada et al., 1990) and plants (Wang and Meresz,
1982), therefore, PAH determination in soil may pro-
vide important information on the environmental pol-
lution state. Characteristic ratio of PAH and PAH
pro®les can be used in qualitative and quantitative
source estimation (Vogt et al., 1987; Yang et al., 1991).
The concentrations and distribution of PAH in Esto-
nia have been studied mainly in water, bottom sedi-
ments, ®sh, etc. (Veldre et al., 1979, 1987; Yegorov et
al., 1989; Trapido and Palm, 1991; Trapido et al., 1992).
No studies have been carried out to assess the accumu-
lation and distribution of PAH in soil. The main aims of
the present study were to assess soil contamination by
PAH in Estonia, to relate PAH compound pro®les to
di€erent types of anthropogenic input and to determine
the regional background PAH levels in soil.
2. Material and methods
2.1. Sampling
The concentrations of PAH in soil and PAH pro®les
were determined in Tallinn, PaÈrnu, Kohtla-JaÈrve, and in
the rural areas: Harjumaa, PaÈrnumaa, and Ida-Virumaa.
Fig. 1. Location of sampling sites for the present study.
The data from the rural areas were used for the estima-
tion of the PAH soil background concentrations in
Estonia. The sampling areas are shown in Fig. 1 and
characterised in Table 1.
A total of 133 soil samples (68 rural and 65 urban
areas) were collected and analysed. Soil samples (0±10
cm upper layer) were collected in September 1996
according to Aamot et al. (1987, 1996). The samples
were collected at least 25 m away from roads in the
urban areas and at least 150 m from the roadside in
the rural ones. Samples were not collected from known
contaminated sites as the territory of power stations and
industrial enterprises, etc.
2.2. Analysis
The samples were dried at room temperature for 2 days,
then at 50 C for 2±3 hours, sieved through a 2-mm mesh
to remove large particles and organic debris, and stored at
5 C prior to analysis. Twenty grams of dry sample were
soaked in 75 ml of hexane (analytical grade, puri®ed
additionally with activated carbon) overnight. The ultra-
sonic extraction procedure twice during 5 minutes
followed (sonicator UZDA-A, Nauchpribor, USSR,
operated at 22‹1.65 kHz; power input was 80 W). The
second extraction was conducted with 50 ml of hexane.
The recovery of PAH from soil obtained using ultrasonic
extraction was comparable to recovery obtained with
 M. Trapido / Environmental Pollution 105 (1999) 67±74 69

Table 1
The sampling sites and the description of the area

Site no. Sampling area Description of area and presupposed PAH sources
(number of samples)

1 Tallinn (34)
2 Tallinn, centre (7)
3 PaÈrnu (16)
4 Kohtla-JaÈrve (15)
5 Maardu (16)
6 Harjumaa (37)
7 PaÈrnumaa (38)
8 Ida-Virumaa (7)
a
According to Statistical Yearbook of Estonia, 1997.
The capital of Estonia, 420 500a inhabitants, heavy trac, industry and heating
Extremely heavy trac, domestic heating
Health resort, 51 800a inhabitants, trac, domestic heating
Industrial area, 53 500a inhabitants, oil-shale thermal treatment industry (KIVITER), chemical
industry, power station, trac
Rural, 20 000a inhabitants, harbour, phosphorite mining (until 1990), trac
Rural, 77 974a inhabitants
Rural, 34 800a inhabitants
Rural, 22 100a inhabitants, oil-shale mining

Soxhlet extraction (Golden and Sawicki, 1975; Trapido,
1995). Combined hexane extracts were evaporated care-
fully to the volume of about 1 ml and then fractionated by
the thin-layer chromatography with aluminium oxide
(TLC grade, Reanal, Hungary). The mobile phase
was hexane±benzene 4:1 (by volume). PAH fraction was
eluted using twice 5 ml of acetone (extra pure grade,
Reachim, Russia). Acetone was evaporated dry at room
temperature and the residue was dissolved in 0.22.0 ml
of acetone (dependent to PAH concentration).
Measurement of PAH concentration was carried out
with high performance liquid chromatography (HPLC;
model 1311, Minsk, Byelorussia). The eluting solvent
was a mixture of acetonitrile-water (both HPLC grade)
93:7 (by volume) with ¯ow rate 8 ml minÿ1. Fluores-
cence detection with initiation wavelength 254 and 298
nm, the range of registration 330±600 nm was used.
Chromatographic column (0.5300 mm) was ®lled with
Silosorb C18 (Chemapol, Czechoslovakia). The coe-
cient of variation for HPLC method was 1.5%. PAH
standards were obtained from Aldrich Chemical Com-
pany. Twelve PAH have been quanti®ed in the sam-
ples: phenanthrene (Ph), anthracene (A), ¯uoranthene
(Fl), pyrene (P), triphenylene (TPh), benzo(a)anthracene
(BaA), chrysene (Chr), benzo(e)pyrene+benzo(b)¯uor-
anthene (BeP), benzo(k)¯uoranthene (BkFl), benzo(a)-
pyrene (BaP), and benzo(ghi)perylene (BghiPer).  PAH
refers to the sum of these 12 compounds. The procedure
described earlier has been checked for recovery e-
ciencies by analyzing soil samples spiked with PAH
standards. Recovery of PAH was in 86±98% range.
Replicate analyses gave an error of ‹10%.
3. Results and discussion
3.1. PAH concentrations
The mean and standard deviations of PAH con-
centrations in soil in di€erent sampling areas are listed
in Table 2. The  PAH values ranged over 4 orders of
magnitude from 11.2 to 153 000 mg/kg. Signi®cant dif-
ferences (at least one order of magnitude) were observed
in  PAH concentrations between rural and urban
areas (see Fig. 2).
PAH concentrations in soil in Tallinn also varied to a
great extent at di€erent sampling points. The  PAH
concentration for Tallinn ranged from 35.5 to max-
imum 26 300 mg/kg. PAH concentrations were sig-
ni®cantly higher in the central part of the city probably
due to intense trac (average value 9015‹6363 mg/kg
dry weight) than in the other parts of the city (compare
data from Table 2). The investigation of snow cover
PAH pollution also indicated enhanced PAH level in
the centre of Tallinn compared to the remote sites of the
city (Trapido et al., 1992). PAH concentration in soil
decreases with increasing distance from the centre of the
city. The decrease of  PAH in north-east direction is
presented in Fig. 3 as a typical example. It declines to
the remote level (200 mg/kg or less) by the outskirts
of the city (8±10 km from the centre).
Transport became the predominant source of envir-
onmental pollution in the city of Tallinn during recent
5±6 years contributing up to 90% of air pollution of
the city (Statistical Yearbook of Estonia, 1997). The
amount of cars has doubled during this period, that is a
unique rate all over the world. As the transport system
is overloaded, frequent (in some locations close to per-
manent) trac jams appear in the centre of the city. At
the same time air pollution load from stationary sources
declined three times due to economical situation (more
than 50% falling-o€ of production). Therefore, trac
could be one of the main reasons for enhanced PAH
concentrations in soil in the centre of the city.
The average PAH concentrations in soil were quite
high in two other cities Ð PaÈrnu and Kohtla-JaÈrve. For
the latter it has been expected, as Kohtla-JaÈrve is an
industrial town (oil-shale thermal treatment, etc.) and
probably the most polluted town in Estonia. High
concentrations of PAH in PaÈrnu (average value 7665
‹4306 mg/kg dry weight) were unexpected as PaÈrnu is a
health resort with minor industrial emissions into the
70 M. Trapido / Environmental Pollution 105 (1999) 67±74

Table 2
The mean concentrations and standard deviations of PAH in soil, mg/kg dry weight

PAH Sampling area (site no.)

Tallinn Tallinn, centre PaÈrnu Kohtla-JaÈrve Maardu Harjumaa PaÈrnumaa Ida-Virumaa

(No. 1) (No. 2) (No. 3) (No. 4) (No. 5) (No. 6) (No 7) (No 8)

Ph 160‹67 680‹628 292‹230 161‹116 18‹8 21‹13 48‹17 61‹45

A 15‹4 69‹53 49‹24 23‹13 1.0‹0.8 0.8‹0.6 2.9‹1.2 2.9‹2.1
Fl 481‹159 2150‹1250 1090‹810 769‹563 22‹16 23‹19 72‹46 44‹24
P 227‹138 762‹550 795‹490 2850‹2278 68‹34 51‹44 142‹98 211‹177
TPh 662‹459 2860‹1900 2540‹1710 2675‹1607 60‹40 52‹29 167‹144 218‹156
BaA 131‹81 536‹382 443‹332 516‹426 10‹6 12‹4.6 22‹15 47‹26
Chr 148‹84 600‹420 507‹420 876‹730 14‹10 15‹9 34‹20 67‹41
BeP 76‹69 289‹161 380‹255 904‹820 8.5‹7.3 12‹5.9 25‹16 31‹17
BkFl 43‹40 162‹125 198‹79 402‹363 4.4‹3.8 5.6‹3.3 12‹6 4.5‹2.5
BaP 106‹60 398‹182 1113‹313 1224‹1090 6.8‹5.1 15‹9 27‹14 31‹23
BghiPer 110‹101 359‹246 233‹196 1996‹1865 25‹23 20‹18 27‹18 51‹30
 PAH (3±4 ring) 1890‹980 7755‹5910 5720‹3440 7870‹5680 188‹103 175‹88 488‹390 652‹485
 PAH (>5 ring) 351‹150 1260‹533 1945‹922 4517‹4140 45‹35 57.5‹29 96‹90 118‹80
 PAH 2200‹1396 9015‹6363 7665‹4306 12390‹9810 233‹185 232‹153 584‹379 770‹595
Number of 34 7 16 15 16 37 8 7
samples

PAH, polycyclic aromatic hydrocarbons; phenanthrene, Ph; anthracene, A; ¯uoranthene, Fl; pyrene, P; triphenylene, TPh; benzo(a)anthracene,
BaA; chrysene, Chr; benzo(e)pyrene+benzo(b)¯uoranthene, BeP; benzo(k)¯uoranthene, BkFl; benzo(a)pyrene, BaP; and benzo(ghi)perylene,
BghiPer.

Fig. 2. Polycyclic aromatic hydrocarbons (PAH) in soil in di€erent

sampling areas. Numbers of sampling areas correspond to those in
Table 1.
atmosphere. The individual domestic heating (mainly
based on wood, coal and peat) is widely used in PaÈrnu.
Trac is also quite intensive in the central part of the
town making its contribution to soil PAH concentra-
tions. These two important sources of PAH are likely to
be responsible for high PAH concentration in soil in
PaÈrnu. PAH concentrations also showed, in general, the
tendency to decrease in direction from the centre of
PaÈrnu to the outskirts.
The study of soil pollution in the town of Kohtla-
JaÈrve indicated very high soil PAH pollution level. An
average  PAH concentration in soil in Kohtla-JaÈrve
(12 390‹9810 mg/kg dry weight) was higher than the
corresponding data from other sampling areas. The
in¯uence of the industrial enterprises on the soil PAH
pollution was quite clear. The average  PAH in soil
Fig. 3.  PAH in soil at various distances from the centre of the city
of Tallinn (north-east direction).  PAH, sum of the compounds;
phenanthrene, Ph; anthracene, A; ¯uoranthene, Fl; pyrene, P; triphe-
nylene, TPh; benzo(a)anthracene, BaA; chrysene, Chr; benzo(e)pyr-
ene+benzo(b)¯uoranthene, BeP; benzo(k)¯uoranthene, BkFl; benzo(a)
pyrene, BaP; and benzo(ghi)perylene, BghiPer.
near the industrial area was twice that in the residential
one.  PAH in 27% of soil samples in Kohtla-JaÈrve
exceeded 4000 mg/kgÐthe intervention value for soil
sanitation set by the Dutch government (Van Brummelen
et al., 1996). These results are quite reasonable and
expected, as oil-shale thermal treatment industry situated
in Kohtla-JaÈrve is known as an important PAH pollu-
tion source (Shabad and Ilnitskii, 1979; Veldre et al.,
1979). Moreover, the highly industrialised north-east is
estimated as one of the most polluted areas in Estonia.
The average PAH concentrations in PaÈrnu, Kohtla-
JaÈrve and also at the central part of Tallinn were higher
 M. Trapido / Environmental Pollution 105 (1999) 67±74
than those reported for the areas contaminated by alu-
minium plant (Vogt et al., 1987), by blast furnace plant
(Van Brummelen et al., 1996) and in soil samples col-
lected 0.5 m from the roadway (Yang et al., 1991). In
23.4% of soils sampled in the urban areas (see Fig. 4) 
PAH exceeded 4000 mg/kg. The data in Table 2 indi-
cates that the average PAH concentration in the cities
was at least one order of magnitude higher than in rural
areas.
PAH concentrations in three rural areas (PaÈrnumaa,
Harjumaa and Ida-Virumaa) varied from 11.2 to 2240
mg/kg. The lowest value was determined in Harjumaa
and the highest in Ida-Virumaa. The latter demonstrates
that PAH pollution level is enhanced not only in the
town of Kohtla-JaÈrve, but also in the surrounding
rural area of Ida-Virumaa. The data for soil PAH
from Maardu were treated separately from the data from
the rest Harjumaa, as there are some di€erences in the
human activities in Maardu and the rest of Harjumaa
(see Table 1), and therefore some di€erences in soil PAH
could be expected. The analysis of the data showed that
there were no di€erences in concentrations or in the
Fig. 4. The distribution of (PAH concentrations in the rural and
urban areas. phenanthrene, Ph; anthracene, A; ¯uoranthene, Fl; pyr-
ene, P; triphenylene, TPh; benzo(a)anthracene, BaA; chrysene, Chr;
benzo(e)pyrene+benzo(b)¯uoranthene, BeP; benzo(k)¯uoranthene,
BkFl; benzo(a)pyrene, BaP; and benzo(ghi)perylene, BghiPer.
71
PAH pattern. The mean  PAH concentrations were
higher in PaÈrnumaa and Ida-Virumaa than in Harjumaa.
Typical soil  PAH concentration derived from
samples from rural areas is estimated at about 100 mg/
kg dry weight. This concentration is typical in the areas
where no anthropogenic pollution sources occur. In
this study 40.3% of soils sampled in the rural areas
have  PAH concentration less than 100 mg/kg (see
Fig. 4). As it has been suggested (Shabad and Ilnitskii,
1979; Edwards, 1983) that the typical endogenous 
PAH in soil, resulting from plant synthesis and natural
®res, is in the range of 1±10 mg/kg. It can be concluded
that typical Estonian soils from rural areas are con-
taminated with PAH above the natural level. This may
be due to long-range atmospheric transport of PAH
from source regions to these remote sites. Taking into
account that the climate conditions in Estonia are
unfavourable for PAH degradation in soil during sub-
stantial part of the year due to low bacterial activity, it
can be assumed that typical soil PAH level is di€erent
when compared with soils in other climates. Therefore,
the typical soil PAH typical level in Estonia can only
be compared with the data from other northern coun-
tries.  PAH from Estonian rural areas is signi®cantly
lower than in south Norway, similar to rural areas in
Wales and twice that in central Norway (Jones et al.,
1989; Aamot et al., 1996). The typical  PAH levels in
Estonia were higher than the target value set by Dutch
government for unpolluted soil (20±50 mg/kg dry
weight; Van Brummelen et al., 1996). This target value
was reached in less than 10% of all samples from
Estonian rural areas.
3.2. PAH pro®les
Fig. 5 presents bar diagrams of PAH as normalised
average concentrations in soil for eight sampling areas.
The main relative proportions appear to be quite con-
stant. Nevertheless, the bar diagrams indicate that the
samples from di€erent sampling sites still have di€erent
patterns.
The three dominant PAH found in soil are pyrene,
triphenylene and ¯uoranthene in all areas under study.
They formed 8±30, 18±35 and 5±25% of the  PAH,
respectively. 3±4 ring PAH dominate in all samples. The
ratio of the 3±4 ring PAH to that of 5±6 ring PAH ratio
varied from 5:1 (in Tallinn and PaÈrnumaa) to 1.7:1 (in
Kohtla-JaÈrve and Ida-Virumaa).
PAH pro®les in all rural areas are quite similar. The
bar diagrams (Fig. 5) show that the samples from the
rural areas have a di€erent PAH pro®le from the soil
samples collected in towns. There are certain di€erences
in PAH pro®les in soil samples from di€erent towns. In
general, PAH pro®les in Tallinn and PaÈrnu are quite
similar. Still, soil samples from PaÈrnu contain relatively
high concentrations of benzo(a)pyrene. Soil from Tallinn
72 M. Trapido / Environmental Pollution 105 (1999) 67±74

Fig. 5. Bar diagram of normalised average polycyclic aromatic hydrocarbons (PAH) concentrations in soil in di€erent sampling areas. Normal-
isation has been done by dividing the average concentration for each PAH by the concentration pyrene (P) in each separate sampling site. PAH:
1, phenanthrene; 2, anthracene; 3, ¯uoranthene; 4, pyrene; 5, triphenylene; 6, benzo(a)anthracene; 7, chrysene; 8, benzo(e)pyrene+benzo(b)¯uor-
anthene; 9, benzo(k)¯uoranthene; 10, benzo(a)pyrene; 11, benzo(ghi) perylene.

has enhanced amount of phenanthrene. PAH pro®le in The important characteristic feature of PAH pro®le in
Kohtla-JaÈrve is di€erent from that in Tallinn and Kohtla-JaÈrve is relatively high concentration of benzo
PaÈrnu, and similar to soil PAH pro®le in rural areas. (ghi)perylene.
 M. Trapido / Environmental Pollution 105 (1999) 67±74
The PAH pro®les have a great importance from the
point of view of potential health e€ects. The samples
from Kohtla-JaÈrve contain relatively high concentra-
tions of heavy PAHÐbenzo(ghi)perylene and benzo(a)
pyrene. Benzo(a)pyrene forms 7±18% of  PAH in soil
samples from PaÈrnu, whilst at the other areas it varies
from 2.9 to 6.5% of the total PAH content. In both,
PaÈrnu and Kohtla-JaÈrve, the soil samples are polluted
with relatively high amount of heavy PAH that are
known to be carcinogenic (have sucient evidence of
carcinogenicity in experimental animals) according to
the estimation of the International Agency for Research
on Cancer (1983).
4. Conclusions
The investigation on the PAH accumulation in soil
showed that Estonian soils are polluted by PAH above
the natural level. PAH concentrations in soil varied
from 11.2 to 153 000 mg/kg dry weight. In the cities, soil
PAH concentrations were quite high. The most PAH
contaminated soil was in Kohtla-JaÈrve. The average
PAH concentration in the cities was at least one order
of magnitude higher than in the rural areas. The typical
 PAH concentration in Estonia may be estimated as
100 mg/kg dry weight, that is higher than the corre-
sponding data from some northern countries. The three
dominant PAH in soil in all sampling areas were found
to be pyrene, triphenylene and ¯uoranthene. Still, the
PAH pattern varied in di€erent sampling areas.
Acknowledgements
The investigation was supported by Estonian Science
Foundation (Grant 2701). The author is deeply grateful
to Mr Heikki Junninen for technical assistance and to
Dr Lidiya Bityukova for her valuable suggestions and
kind help in sampling. Suggestions by two anonymous
referees are gratefully acknowledged.
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