Science of the Total Environment 330 (2004) 249269

Heavy-metal pollution of sediments from Szczecin Lagoon and the

Gdansk Basin, Poland
G.P. Glasbya, P. Szefera,*, J. Geldona, J. Warzochab
a
Medical University of Gdansk, al. Gen. J. Hallera 107, 80-416 Gdansk, Poland
b
Department of Oceanography, Sea Fisheries Institute, ul. 1 Kollataja,
{{ 81-332 Gdynia, Poland

Accepted 5 April 2004

Abstract

Concentrations of Al, V, Mn, Fe, Co, Cu, Ni, Zn, Sr, Mo, Cd, Sb, Pb, Th, U, REE, Na, K, Mg, Ca, Si, P, S, Ti,
Cr and Ba were determined in the -63 mm fraction of bottom sediments of the Szczecin Lagoon and the Gdansk
Basin, Baltic Sea, by ICP-MS, ICP-AES and XRF methods. Sediment samples from the Szczecin Lagoon displayed
somewhat higher concentrations of P, Mn, Cr, Cu and possibly Cd, Pb and Zn in those collected in October 1997
after the exceptional flooding of the Oder River than in those collected in December 2000. The data suggest that the
flood resulted in the enhanced transport of redox-sensitive and anthropogenic elements in the Oder River and their
subsequent redeposition mainly in the western part of Szczecin Lagoon. The sediments of the Szczecin Lagoon also
appear to be the most polluted with heavy metals within the Polish Exclusive Economic Zone (EEZ) of the Baltic
Sea. Cd, Pb, Zn and Cu are anthropogenically enriched in top layers of sediment cores from the Gdansk Basin, but
the decrease of these elements with depth in the core is not systematic. The rare earth element (REE) patterns in
sediments from both these areas do not appear to have been greatly modified during transport from their source into
the southern Baltic. Factor analysis (FA) of the compositional data shows that sediments from Szczecin Lagoon can
be divided into three main groups depending on their composition. It is concluded that clay minerals and organic
matter build aggregates and flocs, which effectively concentrate trace metals and sink down to form a fluffy layer.
2004 Elsevier B.V. All rights reserved.

Keywords: Szczecin Lagoon; Gdansk Basin; Heavy-metal pollution; Rare earth elements; Sediments; Flood

1. Introduction River marks the border between Germany and

The geography of Poland is dominated by the
two main rivers, the Oder and the Vistula, and
their tributaries. In 1995, these rivers discharged
32.9 and and 17.0 km3 of freshwater to the Baltic
Sea, respectively (HELCOM, 1998). The Oder
*Corresponding author. Fax: q48-58-349-3110.
E-mail address: pszef@amg.gda.pl (P. Szefer).
Poland. It is 854 km long and has a catchment
area of 118 860 km2, of which 89% is in Poland
and the remainder in the Czech Republic and
Germany (HELCOM, 1998). The sources of the
Oder and the Vistula Rivers are in Silesia in Poland
and the Czech Republic. These areas form part of
the so-called black triangle of Poland, Czech
Republic and Germany (Markert et al., 1996). The

0048-9697/04/$ - see front matter 2004 Elsevier B.V. All rights reserved.
doi:10.1016/j.scitotenv.2004.04.004
250 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269
main industries in this region are coal mining,
metal mining and metal smelting.
Industrial activity has resulted in heavy-metal
pollution of the bottom and flood plain sediments
of the Oder with maximum concentrations (in mg
gy1) of Zn 6700, Pb 4000, Cu 1800, Ni 350 and
Cd 12 in the Oder River sediments (-63 mm size
fraction; Helios Rybicka, 1996). In 1991, the
surface waters of the upper reaches of the Oder
River were classed as quality class III, the lowest
classification on the Polish water quality classifi-
cation (Helios Rybicka, 1996). However, the dis-
charges of heavy metals, particularly Zn, Pb, Cu,
Cd and Hg, in the Oder decreased by up to 85%
in the period 19881997 (Niemirycz, 1999).
The concentrations of heavy metals in Vistula
River sediments are also very high. In the -63
mm fraction of the sediments, the concentrations
of heavy metals (in mg gy1) were in the range:
Zn 2505300, Pb 57760, Cu 25470, Ni 10
150 and Cd 3140 (Helios Rybicka, 1996). The
highest concentrations of metals were reported in
the sediments of the Przemsza River (a tributary
of the Vistula River) where Zn reached 7000 mg
gy1, Pb 1000 mg gy1 and Cd 200 mg gy1. The
Vistula River drains the Upper Silesian Mining
and Metallurgical Industrial District, which results
in a particularly strong accumulation of metals in
the riverine sediments from this region. In the
Upper Vistula River, )99% of Cd and Pb and )
90% of Zn in the sediment are of anthropogenic
origin over a distance of approximately 200 km.
Concentrations of heavy-metals in estuarine sedi-
ment samples from Gdansk were lower by a factor
of approximately 20 for Cd, 10 for Zn, 5 for Pb
and Cu. The concentrations of Cd were particularly
high and attained some of the highest values
recorded in riverine sediments anywhere in Europe
(Helios Rybicka, 1992, 1993, 1996).
The Oder River discharges into the Baltic Sea
through a lagoon which is divided into the Szcze-
cin Lagoon on the Polish side of the Polish-
German border and the Oder Haff on the German
side of the border. The Oder HaffySzczecin
Lagoon system has a retention time of several
weeks (Beszczynska-Moller, 1999; Meyer and
Lampe, 1999). These lagoons act as natural puri-
fication basins (Lampe, 1999), although with
restricted capacity (Meyer and Lampe, 1999). In
doing so, they become sinks for sediments and
pollutants and, as a result, are now seriously
degraded (HELCOM, 1998). Callaway et al.
(1998) have analyzed sediment cores taken from
high marsh and low marsh areas in Szczecin
Lagoon in an industrial area in the vicinity of the
main channel of the Old Swina River. These
sediments displayed higher concentrations of Zn,
Pb, Cu, Ni and Cd than recorded in four other
coastal wetland areas in northern Europe.
The aim of this study is to evaluate the extent
of heavy-metal pollution of the Szczecin Lagoon
and Gdansk Basin as part of our continuing study
of heavy-metal pollution in the sediments of the
southern Baltic (Szefer et al., 1995a,b, 1996;
Glasby and Szefer, 1998; Renner et al., 1998;
Szefer et al., 1998, 1999; Szefer, 2002).
2. Study areas
2.1. Szczecin Lagoon
The Oder River drains first into the Szczecin
Lagoon and then into the Oder Haff (Fig. 1).
Three different outlets connect the Oder Haffy
Szczecin Lagoon to the Pomeranian Bay in the
Baltic Sea; the Swina, Dziwna and Peene (Pohl et
al., 1998). Approximately 6070% of the water is
transported by the Swina, 1520% by the Dziwna
and 1520% by the Peene. This means that 80
85% of the Oder River water is discharged directly
into the Baltic from Szczecin Lagoon and only
1520% passes through the Oder Haff, Achter-
wasser and Greifswalder Bodden on its way to the
Baltic.
Several studies have reported heavy-metal pol-
lution in sediments of the Oder Haff (Leipe et al.,
1989, 1995; Neumann et al., 1996, 1998; Pohl et
al., 1998; Muller and Heininger, 1999). It has been
suggested that, during seasonal periods of salt-
water inflow from the Baltic Sea, surficial sedi-
ments in the Oder Haff represent a potential source
of heavy metals whereas the sediments in the
Achterwasser represent a potential sink for heavy
metals (Neumann et al., 1998). In spite of this,
the heavy metal contents of the Oder Haff dis-
played the highest average concentrations of
 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269 251

Fig. 1. Schematic map displaying the positions of the sampling sites in Szczecin Lagoon and the Gulf of Gdansk with an inset
showing the locations of these two areas in the southern Baltic.
252 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269

Table 1
Results of an intercomparison of concentrations of major and trace elements (mg gy1 dry wt.), Al, Fe, Ca, Mg, Na, K, P and S
(%) determined in reference sediment materials TILL-1, BCSS-1, MRG-1 and SGR-1 by ICP-MS, ICP-AES and XRF methods

Element Certified Our Recovery Element Certified Our Recovery

value value (%) value value (%)
TILL-1
ICP-MS
Al*q 3.45 3.74 108.4 La 28.0 27.2 97.1
V 103.8 99 104.8 Ce 71 65 90.9
Mnq 1374.0 1420 96.8 Pr* 3.4 4.5 132.5
Feq 4.9 4.8 101.5 Nd 26 29 112.0
Co 17 18 95.5 Sm 5.9 6.0 102.3
Cu 45 47 95.7 Eu 1.3 1.7 129.8
Ni 25 24 103.2 Gd** 2.0 2.5 125
Zn 80 98 82.1 Tb 1.1 0.9 80.3
Sr 274 291 94.1 Dy** 1.9 2.1 110.9
Mo 1.4 2 70.8 Ho** 0.38 0.41 107.4
Cd 0.4 Er 3.6 3.11 86.4
Sb 6.5 7.8 82.7 Tm** 0.17 0.15 90.4
Pb 18 22 80.1 Yb 3.9 3.0 77.6
Th 5.1 5.6 91.9 Lu 0.6 0.4 72.8
BCSS-1
ICP-MS
Alq 5.9 6.3 94.0 Sr 92 96 96.3
V 87 93 93.5 Mo 2.2 1.9 116.2
Mnq 222 229 97.0 Cd 0.3 0.3 112.1
Feq 3.2 3.3 98.2 Sb 0.6 0.59 95.5
Co 12 11 105.0 Pb 21 23 94.2
Cu 16 19 88.3 Th* 0.93 0.88 94.4
Ni 52.2 55.3 94.5 U* 0.24 0.23 97.0
Zn 91 119 76.9
XRF
Si 31.0 30.9 100.3 Ca 0.57 0.54 105.3
Ti 0.44 0.44 99.8 Na 1.98 2.02 98.3
Al 6.29 6.26 100.4 K 1.80 1.80 100.1
Fe 3.22 3.29 97.9 P 0.08 0.07 119.2
Mn 220 310 70.5 S* 0.05 0.06 86.8
Mg 1.41 1.47 95.9
*MRG-1.
**SGR-1.
q
determined by ICP-AES.

heavy-metal pollutants in eight German boddens heavy-metal pollution in sediments of Szczecin

and haffs situated on the Baltic coast (Muller
and
Heininger, 1999). Most of these metals are likely
to be subject to mobilization and redistribution
within the sediments and the water column. The
release or adsorption of trace elements in the
lagoonal sediments is dependent on the rate of
pyrite formation, salt-water inflow, freshwater con-
tribution, and accumulation rate and degradation
rates of organic matter (Muller,
2002). Studies of
Lagoon are more limited than those of the Oder
Haff (Osadczuk and Wawrzyniak-Wydrowska,
1998; Osadczuk, 1999). According to Pempkowiak
et al. (2000), Szczecin Lagoon acts as a trap for
the suspended and dissolved loads carried by the
Oder River.
In 1997, an exceptional flood took place in the
Oder River over a period of approximately 5 weeks
in which approximately 6.5 km3 of additional
 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269
water loaded with nutrients and contaminants was
discharged into the Szczecin Lagoon (Pastuszak et
al., 1998; Siegel et al., 1998; Helios Rybicka and
Strzebonska, 1999; Lehmann et al., 1999; Gre-
lowski et al., 2000). This flood was caused by two
periods of exceptional rainfall during the periods
47 July and 1821 July. However, because of
the high dilution by the flood water, the concen-
trations of heavy-metals and chlorinated organic
contaminants were within the normal range for the
season so that this event was not expected to have
long-lasting, harmful effects on the ecosystems of
the Pomeranian Bay and Baltic Sea (Siegel et al.,
1998). In a comparison of the compositions of
sediments taken in the western and eastern Oder
River in 1995 and in 1997 (-2 mm size fraction),
it was found that the concentrations of Mn and
PCBs increased, the concentrations of Pb
decreased and the concentrations of Cd, Zn and
Ni remained unchanged after the flood (Protasow-
icki et al., 1999). However, the magnitude of the
flood event can be judged from the fact that the
amount of Cu, Pb, Zn, Ni, As, Cr, Cd and Hg
transported on suspended matter during this period
was in the range 3411% of the normal annual
transport of these elements (Muller
and Wessels,
1999).
2.2. Gdansk Basin
The Gdansk Basin is a large anoxic basin with
a maximum depth of 117 m situated seaward of
the Gulf of Gdansk (Fig. 1; Gorlich
et al., 1989;
Szefer et al., 1996; Uscinowicz et al., 1998). The
western part of the gulf is known as Puck Bay.
The surface water salinity in the Gulf of Gdansk
varies between 7.3 and 8.4 but is somewhat
lower near the mouth of the Vistula River (5.5
6.2). The euphotic layers of the Gulf of Gdansk
are well oxygenated but H2S was detected in
waters below 70 m for the first time in 1988.
Sediments vary from coarse sands and gravels to
fine sands at water depths of 3050 m and from
silty clay to clay at greater depths. There are two
distinct zones of sediment deposition in the gulf
separated by a hydrological front. The zone to 10
km from the mouth of the Vistula River is char-
acterized by the rapid deposition of smectites and
253
iron oxyhydroxides. Further offshore, deposition
of illites and chlorites becomes more important.
At water depths greater than 88 m, the sediments
are very dark greenish grey or black muds which
smell strongly of H2S becoming medium to dark
olive-green muds at depths of a few cm within the
sediment column (Szefer and Skwarzec, 1988).
The maximum organic carbon content of the sed-
iments is in excess of 8% (Szczepanska and
Uscinowicz, 1994). The increasing inflow of
industrial and municipal pollution to the Gulf of
Gdansk is derived mainly from the Vistula River,
which transports pollutants from the entire drain-
age area, including the heavy industry belt of
southern Poland. The concentrations of the nutri-
ents, are strongly dependent on season and attain
their maximum values in the waters mainly off the
mouth of the Vistula River. The nutrient-rich
waters can usually be traced more than 15 km
from the mouth of the Vistula River. The influence
of this river is highest during spring and summer
when it extends beyond the gulf and lowest in
autumn and winter when it is restricted to within
a few kilometers (Szefer et al., 1996).
3. Materials and methods
3.1. Sampling
Nine surface sediment samples were collected
from the Szczecin Lagoon by means of a Kajak
corer in October 1997 and a further 11 cores in
December 2000 in order to assess the effect of the
1997 flood event on the contents of heavy metals
and other elements in the sediments. The sediments
are typical muddy sediments enriched in organic
matter up to 1520% or more (dry wt.). In
addition, two sediment cores were taken in Gdansk
Basin in 2000 using a Niemisto corer to study the
distribution of heavy metals and other elements
with depth in the sediment column. Stn P-110 (69
m) is situated in the upper reaches of the halocline
where the sediment is clayey silt and there is
intermittent hypoxia in the near bottom water layer.
Stn G-2 is situated in the deepest part of the basin
(110 m) where the sediment is silty clay and there
is permanent hypoxia and intermittent anoxia in
the near bottom water layer. Fig. 1 shows the
254 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269
locations of the sediment samples from the two
areas. The wet material was stored in plastic bags
in a deeper freezer until chemical analysis could
be carried out.
3.2. Chemical analysis
Bulk samples of sediments were dried at 60 8C,
ground and sieved to pass 63 mm. Two-hundred
milligrams of dried sample were then transferred
to a 50 cm3 teflon beaker and 10 cm3 of conc. HF,
2 cm3 of conc. HNO3 and 1 cm3 of conc. HClO4
added. The beaker was heated on a hot plate for
2 h at 100 8C to remove excess HF. The tempera-
ture of the hot plate was then increased to 230 8C
and the contents of the beaker evaporated to
incipient driness and the beaker removed to cool.
20 cm3 of 3% HNO3 were added and the beaker
returned to the hot plate until the cake had dis-
solved. The digested samples were made up to
100 cm3 with 1% HNO3. 10 cm3 of the sample
solution was spiked with 10 cm3 of an internal
standard solution containing 20 ppb of Ru and Re
for REE analysis and 20 ppb of In and Bi for the
analysis of the other elements. Standard solutions
were run after every 8 samples to monitor and
correct fluctuations of matrix element composition
and instrumental drift. Concentrations of the trace
elements and 14 REE were determined by ICP-
MS using a Fisons VG PlasmaQuad PQ2 Turbo
Plus. Al, Fe and Mn were analyzed by ICP-AES
using a Jobin Yvon 24 Sequential. Five multi-
element standards were used to make up a linear
calibration curve. Major elements were analyzed
by XRF (X-Lab 2000 XRF) using fused glass
beads. Major elements were analyzed by XRF (X-
Lab 2000 XRF) using fused glass beads. Certified
reference materials (TILL-1, MGR-1, BCSS-1,
SGR1) were analyzed in the same way as the
samples in order to estimate the accuracy of the
method. As can be seen in Table 1, element
recoveries were satisfactory as proved by the
analysis of the reference materials.
3.3. Statistical analysis
In order to evaluate the data in more detail, we
have calculated the enrichment factor (EF) for
each element using the formula given by Szefer et
al. (1998):
EFs(Cx yCYb)s y(Cx yCYb)c
where Cx and CYb refer to the concentrations of
elements x and Yb in the surface sediments (s)
and Earths crust (c), respectively. The concentra-
tions of elements in the earths crust are taken
from Riley and Chester (1971). The EFs have
been calculated for the average composition of
sediments from each area (Tables 2, 4, 5 and 7).
EFs41 are generally taken to reflect high levels
of anthropogenic pollution.
We have also calculated the anthropogenic factor
(AF) for each element in the Gdansk Basin sedi-
ment cores using the formula (Szefer and Skwar-
zec, 1988; Szefer et al., 1995b, 1998)
AFsCs yCd
where Cs yCd refer to the concentrations of element
in the surface sediments and at depth of 2530
cm and 4050 cm in the sediment cores P-110
and G-2, respectively.
Correlation analysis and factor analysis of the
concentration data were performed using STATIS-
TICA for Windows, Release 5.0, Copyright Stat-
Soft, Inc. 19841995.
4. Results
4.1. Concentrations of minor, major and REE in
the analysed sediments
4.1.1. Szczecin Lagoon
According to Osadczuk and Wawrzyniak-
Wydrowska (1998), the loss on ignition of samples
of silty sediments from the Szczecin Lagoon was
13.835.2 and concentrations of Corg. ranged from
4.66 to 12.3%. Iron occurs in various chemical
phases of sediments, i.e. as oxides (hematite),
hydroxides (goethite), sulfides (pyrite), sulfates
(e.g. rozenite) and phosphates (e.g. arrojadite).
Chemical speciation of Fe depends on, among
other things, the redox conditions in the sediments.
Concentrations of organic SiO2 and CaCO3 were
between 0.7% and 13.5% and 0.6% and 32.3%,
 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269 255

Table 2
Concentrations of major and trace elements (mg gy1 dry wt.), Al and Fe (%) and Enrichment Factors (EF) in surface sediments
from the Szczecin Lagoon (analyses of all elements by ICP-MS except Al, Mn and Fe determined by ICP-AES)

Stn Al V Mn Fe Co Cu Ni Zn Sr Mo Cd Sb Pb Th U
No.
October 1997
2 4.2 56 2690 5.3 14 133 56 1470 159 1.5 6.4 1.7 180 9.0 3.5
3 3.7 53 4470 4.1 18 81 37 675 164 0.9 3.8 1.2 108 11 2.8
4 3.8 50 3870 4.6 15 111 42 1050 183 1.0 6.9 1.3 145 7.4 1.5
7 4.0 57 1410 4.5 17 90 49 1100 194 1.5 5.8 1.9 156 7.5 2.3
9 3.4 54 1770 4.5 17 92 54 1110 253 1.9 5.3 2.0 166 6.3 1.8
10 3.2 39 1620 4.0 14 69 42 836 237 1.6 4.2 1.6 140 6.6 1.9
11 3.3 43 1130 3.3 12 51 32 651 198 1.2 2.9 1.2 103 7.9 2.2
15 2.7 27 1140 2.0 8.1 24 19 432 201 0.8 2.1 0.7 64 6.4 1.6
17 2.8 42 1710 2.3 6.0 20 14 166 148 0.7 1.0 0.4 40 13 3.8
Average 3.5 47 2200 3.8 13 75 38 832 193 1.2 4.3 1.3 122 8.4 2.4
S.D. 0.5 9.2 1150 1.0 3.8 36 14 375 33 0.4 1.9 0.5 45 2.3 0.8
EF 0.7 0.5 3.5 1.0 0.8 2.0 0.8 18 0.8 1.2 32 9.8 15 1.3 1.3
December 2000
5 3.7 59 2010 4.1 14 90 47 1020 195 0.9 5.5 1.6 133 8.2 2.3
6 3.4 36 1550 2.9 9.8 49 29 665 221 0.8 3.6 1.0 90 7.3 1.8
8 3.8 53 1690 4.0 14 87 45 981 205 1.1 4.9 4.9 125 7.9 2.0
10 3.3 54 2090 4.4 13 80 46 924 221 1.3 4.4 1.3 128 6.3 1.6
12 3.0 34 1230 2.7 8.5 34 24 475 230 0.8 2.4 0.8 70 10 2.2
15 3.4 48 857 2.9 7.1 20 18 256 157 0.6 1.2 0.6 42 16 3.4
16 2.8 36 1130 2.5 7.2 31 21 339 201 2.6 1.9 1.0 67 17 3.7
18 3.5 50 2350 4.4 15 87 47 985 225 1.0 5.0 1.3 142 6.6 1.7
19 4.2 50 1950 4.8 17 103 56 1310 184 1.4 6.3 2.0 167 7.3 2.2
20 3.3 44 1470 4.2 13 72 43 858 210 1.6 3.9 1.5 127 7.1 1.9
21 3.1 39 1430 3.1 11 47 32 568 242 1.0 2.9 1.0 93 8.9 2.0
Average 3.4 46 1610 3.6 12 64 37 762 208 1.2 3.8 1.5 108 9.3 2.3
S.D. 0.4 8.5 454 0.8 3.3 28 13 326 24 0.5 1.6 1.2 38 3.7 0.7
EF 0.7 0.6 2.7 1.0 0.8 1.8 0.8 17 0.9 1.3 30 12 14 1.3 1.3

respectively (Osadczuk and Wawrzyniak-Wydrow-
ska, 1998).
If we consider the average compositions of
surficial sediments from the Szczecin Lagoon in
October 1997 and in December 2000 (Tables 2
4), we see that these sediments are almost identical
in composition for Yb and Al (Al is 2.9% higher
in the 1997 samples). However, several elements
display higher average concentrations in the 1997
samples than in the 2000 samples. In the order of
decreasing enrichment (expressed as a percent-
age) in the 1997 samples relative to the 2000
samples, P (56.7%))Mn (36.6%))Cr (32.0%))
Cu (17.2%))Cd (13.2%)GPb (13.0%))Zn
(9.2%). However, the spread of data (as repre-
sented by the percentage standard deviation) is, in
general, within the limits of analytical error and
much greater for the above-mentioned elements
than for Yb and Al for both the 1997 and 2000
dataset. As can be seen in Tables 2 and 4, there
are variations in the concentrations of some metals
within the lagoon with sediments from the western
part of the lagoon more enriched in Zn, Cu, Pb,
Cd, Mn, Fe and Al than those from the eastern
part of the lagoon.
4.1.2. Gdansk Basin
According to Belzunce-Segarra et al. (2004),
concentrations of Corg. in Gdansk Basin sediment
cores ranged between 6.22% in upper segments of
the cores and 1.54% in the deeper layers. Optical
microscopy showed a dominance of quartz along
with potassium feldspars, plagioclase feldspars,
rock fragments and occasional opaque minerals.
256 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269

Table 3
Concentrations of REE (mg gy1 dry wt.) in surface sediments from the Szczecin Lagoon (analysed by ICP-MS)

Stn La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm Yb Lu
No.
October 1997
2 33 59 8.1 29 5.5 1.2 4.8 0.7 4.0 0.7 2.0 0.3 2.1 0.3
3 34 63 8.4 31 6.6 1.2 5.0 0.8 4.4 0.8 2.3 0.3 2.6 0.4
4 24 43 6.1 21 4.3 1.0 3.8 0.5 3.2 0.6 1.7 0.2 1.7 0.2
7 27 50 6.8 24 4.9 1.1 3.9 0.6 3.6 0.6 1.8 0.3 1.8 0.3
9 23 43 6.1 22 4.4 1.0 3.5 0.5 3.1 0.6 1.6 0.2 1.6 0.2
10 22 41 5.9 20 4.1 0.9 3.3 0.5 2.9 0.5 1.5 0.2 1.6 0.2
11 28 51 7.2 25 4.7 1.0 4.1 0.6 3.6 0.7 1.9 0.3 2.0 0.3
15 19 36 5.4 18 3.6 0.8 2.8 0.4 2.4 0.4 1.3 0.2 1.4 0.2
17 37 69 9.3 34 6.8 1.2 5.5 0.9 5.3 1.0 3.2 0.5 3.5 0.5
Average 27 51 7.0 25 5.0 1.1 4.1 0.6 3.6 0.7 1.9 0.3 2.0 0.3
S.D. 6 11 1.3 5.6 1.1 0.2 0.9 0.2 0.9 0.2 0.6 0.1 0.7 0.1
December 2000
5 25 47 6.6 23 4.8 1.0 3.8 0.6 3.5 0.6 1.8 0.2 1.8 0.2
6 22 41 6.0 20 4.1 0.9 3.2 0.5 3.0 0.5 1.5 0.2 1.5 0.2
8 24 44 6.3 22 4.4 1.0 3.6 0.5 3.3 0.6 1.8 0.2 1.7 0.2
10 21 39 5.7 19 3.9 0.9 3.2 0.5 2.8 0.5 1.5 0.2 1.4 0.2
12 28 51 7.3 26 5.2 1.0 4.1 0.6 3.5 0.6 1.9 0.3 2.0 0.3
15 42 80 11 40 8.0 1.2 6.1 0.9 5.5 1.0 2.9 0.4 3.2 0.5
16 43 81 11 40 7.8 1.2 6.0 0.9 5.0 0.9 2.6 0.4 2.9 0.4
18 22 40 5.9 20 4.1 1.0 3.3 0.5 2.9 0.5 1.6 0.2 1.5 0.2
19 26 48 6.7 23 4.8 1.1 3.8 0.6 3.6 0.6 1.8 0.3 1.8 0.3
20 23 43 6.2 21 4.3 0.9 3.5 0.5 3.0 0.6 1.6 0.2 1.6 0.2
21 28 51 7.2 24 4.9 1.0 3.9 0.6 3.7 0.6 1.9 0.3 1.9 0.3
Average 28 51 7.2 25 5.1 1.0 4.0 0.6 3.6 0.6 1.9 0.3 1.9 0.3
S.D. 8 15 1.8 7.5 1.4 0.1 1.0 0.1 0.9 0.2 0.4 0.07 0.6 0.09

Chlorite occurred rarely. Fragments of diatoms and
plants debris were common.
For the Gdansk Basin sediments, it is seen that
the spread of data (as represented by the percent-
age standard deviation of element concentrations
in the whole core) was, in general, much greater
for the anthropogenic and redox-sensitive elements
than for Yb and Al in the two cores (Tables 5
7).
Plots of the element concentrations in the two
sediment cores revealed different vertical distribu-
tion patterns (Figs. 2 and 3). In core P-110, for
example, Cd, Zn, Pb, Cu, Sb showed steadily
decreasing concentrations with depth in the core
but with a pronounced peak at a depth of 15 cm.
Mn, however, showed a pronounced minimum
between 5 and 20 cm in the core. In core G-2, Cd,
Zn, Pb, Sb and Cu all decreased with depth,
although Zn, Pb and Cu displayed peaks at a depth
of 5 cm. Mn, however, increased steadily with
depth in the core.
4.2. Enrichment factors of elements in Szczecin
Lagoon
Fig. 4a shows a significant enrichment of S, Cd,
Zn, Pb, Sb, P, Mn and Cu in the surficial sediment
samples taken from Szczecin Lagoon. Based on
the mean EFs, enrichment of the P and Mn in the
surficial sediment samples taken from Szczecin
Lagoon in October 1997 was greater than in
samples taken in December 2000 (Tables 2 and
4). These elements also showed a greater spread
in values compared to elements such as Yb and
Al, incorporated in the lithogenous fraction of the
sediment. By contrast, S and Ca exhibit significant
enrichment in the surficial sediments collected in
December 2000 compared to those from October
 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269 257

Table 4
Concentrations of major elements (%), Cr, Ni and Ba (mg gy1 dry wt.) and Enrichment Factors (EF) in surface sediments of the
Szczecin Lagoon (analysed by XRF)

Stn Na Mg Al Si P S K Ca Ti Cr Mn Fe Ni Ba
No.
October 1997
2 0.73 0.47 4.07 26.5 0.59 0.65 1.34 2.89 0.36 160 0.26 5.30 -50 704
4 1.00 0.49 3.41 20.1 0.59 0.49 1.05 5.67 0.25 120 0.35 4.20 -50 542
11 0.95 0.59 3.02 25.8 0.26 1.49 1.28 5.87 0.39 90 0.11 3.20 -50 305
17 0.59 0.51 2.77 33.3 0.43 0.41 1.35 3.45 0.90 140 0.15 2.50 -50 214
Average 0.82 0.52 3.32 26.4 0.47 0.76 1.26 4.47 0.48 128 0.22 3.80 441
S.D. 0.19 0.05 0.57 5.4 0.16 0.50 0.14 1.52 0.29 30 0.11 1.22 223
EF 0.4 0.3 0.6 1.2 6.1 38 0.7 1.4 1.1 1.7 3.2 0.9 1.4
December 2000
5 0.58 0.61 3.99 24.0 0.40 0.66 1.28 7.08 0.30 110 0.21 4.50 -50 511
6 0.65 0.47 3.29 24.8 0.27 0.96 1.30 8.38 0.23 70 0.15 3.00 -50 422
12 0.64 0.56 2.93 24.3 0.21 0.60 1.23 10.07 0.31 80 0.13 2.70 -50 341
15 0.61 0.61 3.24 29.6 0.26 1.21 1.41 5.30 0.59 100 0.09 2.90 -50 254
18 0.64 0.77 3.91 20.8 0.36 1.04 1.15 10.66 0.28 140 0.28 5.30 -50 566
21 0.95 0.64 2.92 20.9 0.29 0.70 1.08 10.41 0.29 80 0.14 3.20 -50 327
Average 0.68 0.61 3.38 24.1 0.30 0.86 1.24 8.65 0.33 97 0.17 3.60 404
S.D. 0.14 0.10 0.47 3.2 0.07 0.24 0.12 2.14 0.13 26 0.07 1.05 119
EF 0.4 0.5 0.6 1.3 4.5 51 0.8 3.1 0.9 1.5 2.5 0.9 1.4

Table 5
Concentrations of major and trace elements (mg gy1 dry wt.), Al and Fe (%) and Enrichment Factors (EF) in sediment cores from
the Gdansk Basin (analyses all elements by ICP-MS except Al, Mn and Fe analysed by ICP-AES)

Stn Sediment Al V Mn Fe Co Cu Zn Ni Sr Mo Cd Sb Pb Th U
No. Depth
(cm)
P-110 02.5 4.8 71 399 2.8 8.9 37 139 30 106 1.1 1.2 0.7 52 10 2.8
2.55 4.4 51 308 2.8 6.7 27 108 22 98 1.4 1.2 0.6 47 9.0 2.7
510 4.9 61 309 3.0 7.5 31 136 27 97 1.6 1.2 0.6 62 9.2 2.7
1015 4.7 61 305 2.9 7.9 33 157 26 102 1.3 1.5 0.8 77 9.2 2.7
1520 4.2 49 311 2.4 5.9 20 90 19 92 1.5 0.7 0.7 54 9.8 2.5
2025 4.4 48 332 2.5 6.4 15 65 19 94 1.8 0.3 0.5 38 11 2.5
2530 4.9 78 384 3.1 9.0 19 61 25 98 2.8 0.3 0.6 28 9.9 2.6
Average 4.6 60 335 2.8 7.5 26 108 24 98 1.6 0.9 0.7 51 9.7 2.7
S.D. 0.3 12 40 0.2 1.2 8.2 38 4.0 4.9 0.6 0.5 0.1 16 0.6 0.1
EF 0.7 0.6 0.5 0.7 0.4 0.6 2.0 0.4 0.3 1.4 6.0 4.3 5.3 1.3 1.0
G-2 02.5 5.1 94 329 3.9 16 56 228 46 110 34 1.7 2.2 67 8.8 9.4
2.55 6.5 108 418 4.6 18 57 248 47 88 15 1.5 1.9 90 11 6.1
510 7.0 103 515 5.1 18 52 219 46 87 6.4 1.1 1.8 90 12 5.0
1015 6.3 107 471 5.0 17 51 216 45 87 6.7 1.2 2.0 90 11 4.8
1520 6.8 113 632 5.3 19 49 211 47 100 5.8 1.2 2.2 85 12 4.6
2025 7.5 118 816 5.5 17 43 170 48 92 4.1 0.6 1.8 73 12 3.9
2530 7.0 117 757 5.6 21 39 139 48 107 8.1 0.5 1.5 56 13 4.2
3040 7.3 123 978 6.1 22 38 119 49 107 5.2 0.6 1.2 46 13 4.2
4050 7.4 105 1340 6.4 19 38 115 46 103 4.6 0.5 1.0 45 13 4.4
Average 6.7 110 695 5.3 18 47 185 47 98 9.9 1.0 1.7 71 12 5.2
S.D. 0.7 8.8 319 0.8 1.8 7.6 50 1.3 9.7 9.4 0.5 0.4 19 1.3 1.7
EF 1.0 1.0 0.9 1.2 0.9 1.1 3.3 0.8 0.3 8.3 6.3 11 7.1 1.5 2.4
258 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269

Table 6
Concentrations of REE (mg gy1 dry wt.) in sediment cores from the Gdansk Basin (analysed by ICP-MS)

Stn Sediment La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm Yb Lu
No. Depth
(cm)
P-110 02.5 29 55 7.7 27 5.4 1.1 4.2 0.7 3.9 0.7 2.2 0.3 2.2 0.3
2.55 28 51 7.4 26 5.1 1.1 4.1 0.7 3.9 0.7 2.1 0.3 2.1 0.3
510 28 53 7.4 26 5.3 1.1 4.2 0.7 4.1 0.8 2.2 0.3 2.2 0.3
1015 27 51 7.3 25 5.2 1.1 4.1 0.6 3.9 0.7 2.1 0.3 2.2 0.3
1520 30 57 7.9 29 5.6 1.1 4.5 0.7 4.2 0.8 2.3 0.3 2.5 0.3
2025 31 60 8.3 29 5.9 1.1 4.6 0.7 4.3 0.8 2.4 0.4 2.4 0.4
2530 31 59 8.1 29 5.8 1.2 4.6 0.7 4.2 0.8 2.4 0.3 2.4 0.3
Average 29 55 7.7 27 5.5 1.1 4.3 0.7 4.1 0.7 2.2 0.3 2.3 0.3
S.D. 1.6 3.7 0.4 1.7 0.3 0.04 0.2 0.03 0.2 0.04 0.1 0.02 0.1 0.03
G-2 02.5 28 50 6.9 24 5.0 1.0 4.0 0.6 3.6 0.7 2.0 0.3 1.8 0.2
2.55 34 63 8.5 30 5.8 1.2 4.7 0.7 4.5 0.8 2.4 0.3 2.3 0.3
510 38 69 9.2 34 6.9 1.4 5.2 0.8 4.8 0.9 2.6 0.4 2.5 0.4
1015 36 64 8.7 31 6.1 1.3 5.0 0.8 4.8 0.9 2.5 0.3 2.3 0.3
1520 38 68 9.1 33 6.2 1.3 5.2 0.8 4.8 0.9 2.6 0.4 2.5 0.4
2025 38 68 9.4 33 6.8 1.4 5.4 0.8 4.9 0.9 2.6 0.4 2.4 0.3
2530 39 72 9.6 34 6.8 1.4 5.5 0.8 5.1 0.9 2.8 0.4 2.6 0.3
3040 39 70 9.4 35 7.0 1.4 5.5 0.8 5.1 0.9 2.7 0.4 2.6 0.4
4050 39 69 9.4 35 6.8 1.5 5.6 0.9 5.2 0.9 2.8 0.4 2.6 0.3
Average 36 66 8.9 32 6.4 1.3 5.1 0.8 4.7 0.9 2.5 0.4 2.4 0.3
S.D. 3.6 6.8 0.8 3.4 0.7 0.1 0.5 0.1 0.5 0.1 0.2 0.04 0.2 0.04

Table 7
Concentrations of major elements (%), Cr, Ni and Ba (mg gy1 dry wt.) and Enrichment Factors (EF) in sediment cores from the
Gdansk Basin (analysed by XRF)

Stn Sediment Na Mg Al Si P S K Ca Ti Cr Mn Fe Ni Ba
No. Depth
(cm)
P-110 02.5 1.22 1.29 4.93 28.6 0.15 0.32 2.11 1.37 0.35 70 0.03 2.79 -50 332
2.55 1.03 1.19 4.55 30.2 0.12 0.41 2.08 1.48 0.36 70 0.03 2.84 -50 346
510 1.20 1.31 4.69 29.3 0.12 0.45 2.07 1.48 0.36 70 0.03 2.97 -50 327
1015 1.02 1.18 4.68 30.3 0.11 0.51 2.04 1.35 0.37 78 0.03 2.86 -50 342
1520 0.93 1.15 4.45 32.0 0.11 0.75 2.08 1.56 0.40 61 0.03 2.54 -50 339
2025 1.01 1.21 4.66 32.7 0.11 0.62 2.05 1.52 0.38 62 0.03 2.55 -50 358
2530 1.00 1.22 5.02 30.8 0.12 0.86 2.18 1.36 0.40 69 0.04 3.11 -50 355
Average 1.06 1.22 4.71 30.6 0.12 0.56 2.09 1.45 0.37 69 0.03 2.81 343
S.D. 0.11 0.06 0.20 1.4 0.02 0.19 0.05 0.09 0.02 6 0.003 0.21 11
EF 0.6 0.8 0.7 1.4 1.6 28 1.1 0.4 0.9 0.9 0.5 0.7 1.1
G-2 1015 1.44 1.41 6.86 24.0 0.15 1.29 2.37 0.49 0.33 86 0.06 5.14 -50 339
1520 1.13 1.28 6.64 21.6 0.13 1.01 2.29 0.46 0.32 76 0.07 4.23 -50 316
4050 1.11 1.39 7.16 23.2 0.17 1.74 2.53 0.64 0.35 88 0.12 5.94 -50 343
Average 1.23 1.36 6.88 22.9 0.15 1.35 2.40 0.53 0.34 83 0.08 5.10 333
S.D. 0.19 0.07 0.26 1.2 0.02 0.37 0.12 0.09 0.02 6 0.03 0.86 14
EF 0.6 0.8 1.0 1.0 1.8 62 1.2 0.2 0.7 1.0 1.0 1.2 1.0
 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269 259

Fig. 2. Distribution patterns of element concentrations in mg gy1 except Al and Fe in % with depth (mm) in sediment core P-110
from the Gdansk Basin.
260 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269

Fig. 3. Distribution patterns of element concentrations in mg gy1 except Al and Fe in % with depth (mm) in sediment core G-2
from the Gdansk Basin.
 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269
Fig. 4. Enrichment Factors (EFs) for elements in sediments
from: (a) Szczecin Lagoon based on the average compositions
of samples collected in October 1997 and December 2000 and
(b) the Gdansk Basin based on the average compositions of
samples from Cores G-2 and P-110.
1997. In previous publications, we have shown
that the elements P, Cu, Pb, Sb, Cd and Zn are
anthropogenically enriched in the sediments from
the southern Baltic (Szefer et al., 1995a,b, 1996,
1998, 1999; Szefer, 2002). Mn, Fe and Co are
known to be redox-sensitive elements which can
migrate under the influence of changes in redox
conditions of the environment (Glasby and Schulz,
1999).
4.3. Enrichment factors of elements in the Gdansk
Basin
There was a significant enrichment of S, Cd,
Pb, Sb (core P-110) and S, Sb, Mo, Pb and Cd
261
(core G-2) in the surficial sediment samples taken
from the Gdansk Basin (Fig. 4b). The AFs
reached the highest values for Cd (3.7), Zn (2.3),
Cu (1.9) and Pb (1.9) in core P-110 and for Mo
(7.4), Cd (3.4), Sb (2.2), U (2.1) and Zn (2.0) in
core G-2. The AFs for the REE and Al were F1.
The data from the Gdansk Basin sediment cores
are in accordance with previous findings that Cd,
Pb, Zn and Cu are anthropogenically enriched in
sediment cores from the Gulf of Gdansk and Puck
Bay (AFs)1) and that these elements decrease
with depth in the sediment column (Szefer and
Skwarzec, 1988; Szefer et al., 1995b, 1998; Usci-
nowicz et al., 1998). However, the decrease with
depth is not systematic in the cores studied here
and the element concentrations display maxima at
certain depths within the sediment column (Figs.
2 and 3).
Concentrations of major elements such as K,
Na, Ca, Mg and P were similar to those reported
earlier for surface sediments and sediment cores
of the southern Baltic (Szefer and Skwarzec, 1988;
Szefer et al., 1995a, 1996, 1998).
4.4. REE in the study areas
NASC-normalized REE patterns for Szczecin
Lagoon and Gdansk Basin sediments are presented
in Fig. 5. The Szczecin Lagoon data give almost
identical plots for the average 1997 and 2000 data,
although there is a relatively large spread in the
concentrations of each element within each dataset
(S.D.)20%). The plots for the Gdansk Deep
sediments are very similar to those of the Szczecin
Lagoon sediments except that samples from Stn
G-2 have higher concentrations on average than
those from Stn P-110. The spread in the concen-
trations of each element within each core is rela-
tively small (-10%). In fact, these plots of
average REE concentrations are quite similar to
those previously presented for sediments from the
Vistula Lagoon (Szefer et al., 1999).
4.5. Statistical relationships
Concentration data for sediments from Szczecin
Lagoon were processed using correlation analysis
(Table 8) and factor analysis (Fig. 6).
262 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269

Fig. 5. Plots of the average North American Shale Composite (NASC)-normalized REE data for sediments from each of the study
areas. NASC concentration data taken from McLennan (1989); all values in mg gy1 : La 32, Ce 73, Pr 7.9, Nd 33, Sm 5.7, Eu 1.24,
Gd 5.2, Tb 0.85, Dy 5.8, Ho 1.04, Er 3.4, Tm 0.5, Yb 3.1 and Lu 0.48.

4.5.1. Interelemental correlations associated with biogenic material in the lagoonal

As can be seen in Table 8, elements such as Th,
U, Si and Ti are strongly correlated (P-0.01)
with Yb, the reference element for the lithogenous
component, in Szczecin Lagoon sediments and
have average EFM Yb;1. Elements such as Cu, V,
S, P, Fe and Al do not show any correlation with
Yb; moreover, Cd, Sb, Pb and Zn, exhibit negative
correlations with Yb. This means that concentra-
tions of these elements are not directly controlled
by continental weathering. It should be emphasised
that Cu, and especially Cd, Sb, Pb and Zn, are
significantly enriched relative to crustal material
(EFMYb)1). A significant proportion of these ele-
ments is thought to be bound with particles of
fluffy material which build aggregates with
organic matter (Loffler
et al., 2000).
Elements such as Na and Mg as well as Co, Ni,
Sr, Ba and Ca are not correlated or are correlated
negatively with Yb and show average EFM YbF1.
This implies that a significant fraction of these
elements is associated with phases other than
crustal material. Concentrations of Ba, Ca and
especially Sr show negatively-related trends to the
Yb content. These elements are therefore possibly
sediments.
4.5.2. Distribution of metals based on factor
analysis
In order to reduce the relatively large number
of variables to a smaller number of orthogonal
factors, the original data obtained were processed
by multivariate statistical methods. Factor analysis
(FA) was performed on the 20 samples from
Szczecin Lagoon. Three factors (F1-F3) were
obtained which explained 86.2% of the total vari-
ance and eigenvalues accounted for 9.4, 3.0 and
1.4, respectively. Fig. 6a shows a plot of F1 vs.
F2 for object scores of 20 sediment samples
(station numbers 221) and Fig. 6b a plot of F1
vs. F2 for object scores of 16 elements.
A plot of the object samples shows a clustering
of the samples into three main areas, each corre-
sponding to a geographically distinct zone (Fig.
6a). Samples from the western part of the Szczecin
Lagoon (samples 25, 79, 19 located in the right
part of the plot) have the highest scores of F1 and
are the most influenced by the riverine input.
These samples are generally characterized by the
 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269
highest concentrations of Cd, Pb, Cu, Zn, Co, Ni,
V, Mn and Sb as shown in Fig. 6b. Loffler et al.
(2000) have previously shown that clay minerals
and organic matter (OM) build aggregates and
flocs which concentrate trace metals and then sink
to form a fluffy layer. The element distribution
patterns presented here suggest that this fluffy
layer is deposited mainly in the western part of
Szczecin Lagoon.
263
In contrast, samples from eastern part of the
lagoon (samples 6, 11, 12, 1517, 21) located in
the left part of the plot) display low scores of F1
(Fig. 6a). These low values are attributed to the
enrichment of elements of terrigenous origin such
as Yb, Th, U and Sr (Fig. 6b).
Samples 10 and 20 (identified in the central
part of the plot) are located in north-western part
of the lagoon and appear to be transitional in
composition (Fig. 6a), possibly associated with
Mo (Fig. 6b).
5. Discussion
5.1. Enrichment of elements in Szczecin Lagoon
The exceptional Oder River flood took place in
July 1997 but its effects lasted throughout August
1997 (Muller-Navarra
et al., 1999). One feature of
the flood was a sudden drop in the oxygen content
of the Oder River water to concentrations as low
as 2 mg dmy3 (Niemirycz, 1999). Moreover, the
contribution of Oder Lagoon organic matter
decreased from 50 to approximately 30% (Miltner
and Emeis, 2000) and the fluffy layer contained
a very high proportion of branched fatty acids of
bacterial origin (Laima et al., 1999). Another
feature was the enhanced transport of heavy metals
and other pollutants adsorbed on particulate matter
Fig. 6. (a) Plot for object scores of factors F1 and F2 for 20
sediment samples from Szczecin Lagoon, (b) Plot for loadings
of factors F1 and F2 for 16 elements from Szczecin Lagoon
and (c) Schematic map showing the distribution of geo-
chemical facies within Szczecin Lagoon obtained by Osadczuk
and Wawrzyniak-Wydrowska (1998). According to these
authors, spatial variations are illustrated by groupings of points
corresponding to geochemical facies in three sectors of the
lagoon, namely facies B (B1qB2) with high contents of OM,
amorphous SiO2 and heavy metals (samples 25, 79, 19);
facies A1aqA2 with very low contents of OM, amorphous
SiO2, heavy metals and CaCO3 (samples 6, 11, 1517, 21)
and facies A1b1 with intermediate contents of the OM, amor-
phous SiO2, heavy metals and CaCO3 and transitional between
B and A1aqA2 facies (samples 10, 20). Clustering of the
loadings reflects the statistically significant relations of Al, Fe,
Cd, Pb, Cu, Zn, Co, Ni, V, Mn and Sb to facies B (B1qB2),
Yb, Th, U and Sr to facies A1aqA2 and Mo to facies A1b1.
The numbers and the locations of the facies and their chemical
compositions are taken from Osadczuk and Wawrzyniak-
Wydrowska (1998).
 264

Table 8
Correlation coefficients calculated for concentrations of selected chemical elements in surface sediments of the Szczecin Lagoon (Ns10, P-0.05a, P-0.01b)

Na Mg Si P S K Ca Ti Cr Ba Al V Mn Fe Co Cu Ni Zn Sr Mo Cd Sb Pb Th U Yb

Na 1.00
Mg y0.08 1.00
Si y0.51 y0.35 1.00
P 0.20 y0.37 y0.07 1.00
S 0.10 0.41 0.01 y0.54 1.00
K y0.65a y0.28 0.86b y0.17 0.26 1.00
Ca 0.03 0.60 y0.66a y0.58 0.12 y0.56 1.00
Ti y0.36 y0.15 0.89b 0.03 y0.13 0.58 y0.58 1.00
Cr y0.17 0.00 0.21 0.79a y0.32 0.12 y0.55 0.34 1.00
Ba 0.07 y0.05 y0.51 0.67a y0.20 y0.26 y0.05 y0.59 0.53 1.00
Al 0.14 y0.17 y0.33 0.66a 0.01 y0.03 y0.33 y0.48 0.47 0.88b 1.00
V y0.09 0.14 y0.07 0.66a y0.07 0.09 y0.43 y0.06 0.68a 0.64a 0.77b 1.00
Mn 0.33 y0.23 y0.45 0.88b y0.50 y0.52 y0.22 y0.31 0.58 0.74a 0.63a 0.52 1.00
Fe 0.24 0.03 y0.49 0.74a y0.10 y0.28 y0.19 y0.49 0.61 0.94b 0.92b 0.77b 0.76a 1.00
Co 0.40 0.23 y0.75a 0.53 0.01 y0.55 0.13 y0.70a 0.34 0.84b 0.75a 0.62 0.70a 0.89b 1.00
Cu 0.26 y0.11 y0.51 0.78b y0.23 y0.33 y0.19 y0.53 0.56 0.96b 0.90b 0.71a 0.82b 0.98b 0.90b 1.00
Ni 0.20 0.12 y0.59 0.59 y0.08 y0.33 0.01 y0.63a 0.46 0.95b 0.85b 0.70a 0.65a 0.95b 0.94b 0.95b 1.00
Zn 0.22 y0.07 y0.53 0.66a y0.13 y0.28 y0.10 y0.61 0.48 0.97b 0.90b 0.66a 0.71a 0.96b 0.90b 0.98b 0.98b 1.00
Sr 0.22 0.43 y0.73a y0.53 0.13 y0.61 0.95b y0.70a y0.61 0.03 y0.25 y0.48 y0.17 y0.12 0.23 y0.08 0.11 0.03 1.00
Mo 0.47 y0.11 y0.33 0.51 0.06 y0.19 y0.22 y0.40 0.42 0.69a 0.65a 0.40 0.43 0.75a 0.69a 0.76a 0.78b 0.80b 0.00 1.00
Cd 0.30 y0.09 y0.64a 0.71a y0.24 y0.45 y0.05 y0.65a 0.41 0.93b 0.85b 0.64a 0.85b 0.92b 0.92b 0.97b 0.92b 0.95b 0.06 0.65a 1.00
Sb 0.25 0.05 y0.57 0.50 0.01 y0.27 y0.01 y0.68a 0.32 0.88b 0.84b 0.67a 0.56 0.89b 0.92b 0.91b 0.97b 0.95b 0.13 0.78b 0.89b 1.00
Pb 0.31 0.02 y0.60 0.66a y0.10 y0.38 y0.05 y0.63a 0.47 0.95b 0.85b 0.64a 0.73a 0.96b 0.94b 0.98b 0.98b 0.99b 0.09 0.82b 0.95b 0.95b 1.00
Th y0.39 y0.10 0.76a y0.20 0.00 0.62 y0.42 0.77b 0.04 y0.61 y0.36 y0.08 y0.49 y0.51 y0.78b y0.61 y0.68a y0.66a y0.60 y0.55 y0.70a y0.70a y0.72a 1.00
U y0.45 y0.29 0.89b 0.17 y0.13 0.78b y0.73a 0.82b 0.46 y0.25 y0.07 0.19 y0.28 y0.18 y0.55 y0.23 y0.31 y0.26 y0.79 y0.06 y0.42 y0.34 y0.34 0.77b 1.00
Yb y0.38 y0.07 0.86b y0.03 y0.07 0.60 y0.54 0.96b 0.30 y0.59 y0.42 y0.02 y0.36 y0.47 y0.73a y0.55 y0.64b y0.63a y0.71a y0.45 y0.68a y0.70a y0.66a 0.91b 0.85b 1.00
G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269
 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269
during the flood relative to the annual transport of
these elements (Muller
and Wessels, 1999; Witt
and Siegel, 2001). The heavy metals were probably
leached from mine workings, mine spoils and
smelters in the upper reaches of the Oder River
which were submerged during the flooding (Helios
Rybicka, 1996; Niemirycz, 1999). In addition, sub-
stantial amounts of municipal waste were taken up
during the flood. However, as shown by Helios
Rybicka (1996), the heavy-metal contents in the
Oder River sediments decline along the river from
their highest values in Upper Silesia. On this basis,
only a small proportion of the heavy metals
released during the flood would have been trans-
ported as far as Szczecin Lagoon. However, the
flood was a dramatic event and it is possible that
high concentrations of suspended material could
have been transported to the lagoon. The ratios of
the loads of heavy metals in the Oder River during
the flood to those during the entire year have been
determined to be: Cu (33.9%), Pb (28.1%), Zn
(25.9%) and Cd (11.3%) (Muller and Wessels,
1999). Interestingly, this is almost the same order
as the enrichment of these elements in the 1997
samples relative to the 2000 samples (see above).
Element concentrations in sediment samples
from Szczecin Lagoon taken in October 1997 and
in December 2000 do not represent a time-series
analysis. Nonetheless, taken in conjunction with
other information, the flood does appear to have
resulted in the enhanced transport of redox-sensi-
tive and anthropogenic elements in the Oder River
and the subsequent redeposition of these elements
in the sediments of Szczecin Lagoon such that
elevated concentrations were still recorded in the
sediments 5 weeks after the flood waters had
subsided. These concentrations then declined sig-
nificantly over the next 3 years. The Oder Haffy
Szczecin Lagoon is well known to act as a
geochemical trap for Mn, which is highly concen-
trated in surface sediments from this area (Leipe
et al., 2000).
If the heavy-metal concentrations are compared
with those in sediments from other parts of the
southern Baltic, it is seen that the sediments
collected from Szczecin Lagoon in December 2000
display significantly higher in Zn and Pb but
somewhat lower in Cu and Cd than the sediments
265
from the Gulf of Gdansk (which in turn are higher
than those from Puck Bay and the Vistula Lagoon;
Glasby and Szefer, 1998). On this basis, we can
say that the Szczecin LagoonyOder Haff is the
area most polluted with heavy metals, especially
Zn, Pb and Cd within the Polish EEZ.
5.2. Enrichment of elements in the Gdansk Basin
The pronounced peaks of Pb, Cd, Cu and Zn
plus Sb at a depth of 15 cm in the sediment
column in core P-110 (Fig. 2) could represent the
occurrence of a sulfide-rich horizon. The decrease
in concentration of Pb in the upper layers of core
G-2 (Fig. 3) could indicate a lower input of Pb at
this site during the last few years. Irregular vertical
distributions of U and Th in core G-2 illustrated
in Fig. 3 are similar to those obtained for sediment
core from the same sampling site collected in July
1980 (Szefer and Skwarzec, 1988). According to
these authors, Th correlated significantly with Al
and Fe (P-0.01) indicating that crustal weather-
ing may be the main source of these elements in
the sediment cores (Szefer and Skwarzec, 1988).
This observation is supported by the great similar-
ity of both Th and Al distributions in sediment
core G-2 (Fig. 3). As regards U, its vertical
distribution is similar to that of Mo (Fig. 3) which
suggests that redox processes are responsible for
the deposition of both these elements in the
Gdansk Basin (G-2). Prange and Kremling (1985)
have suggested that Mo is most probably removed
from the Baltic Sea waters by adsorption on
particulate organic matter. This finding is support-
ed by the similarity of their redox chemistries.
Based on investigations of long cores from the
Baltic deep basins, Kunzendorf et al. (2001) have
reported that Mo is correlated with organic carbon
and total nitrogen. The authors have suggested that
Mo may be connected with algal blooms because
this element is essential for cyanobacterial uptake
of nitrogen. It is thought that algal remnants with
increased concentrations of Mo are transported to
the seafloor attached to particulate matter. Under
anoxic conditions, the Mo is then deposited in the
form of molybdenite, which remains stable after
burial (Kunzendorf et al., 2001). The distribution
pattern of V shows considerable differences com-
266 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269
pared to the patterns of U and Mo. According to
Prange and Kremling (1985), the abundance of V,
in contrast to that of U and Mo, seems to be
controlled mainly by scavenging by terrigenous
andyor biogenic suspended matter during transport
through the Baltic Sea. Elements such as Mo, V,
Cu and Cd are enriched in laminated sediments
from different basins of the Baltic Sea that have
accumulated under anoxic conditions (Sohlenius,
1996; Sohlenius and Westman, 1998; Sternbeck et
al., 2000; Sohlenius et al., 2001).
Data of sequential extraction analysis of trace
elements in the Gdansk Bay sediments showed
that metals such as Fe, Mn and Zn are associated
with the oxide fraction whereas Pb is associated
with both the organic and oxide fractions (Belzun-
ce-Segarra et al., 2004). Cu, Ni, Co and Cr are
generally present in the residual fraction. Metals
bound to oxides (Mn, Fe, Zn) and organic ligands
(Pb) may be easily remobilized under different
redox conditions in contrast to those in the residual
fraction, i.e. Cu, Cr, Co and Ni.
5.3. Distribution patterns of REE in the study
areas
The REE distribution patterns illustrated in Fig.
5 are not exactly shale-like but display slight
depletions of heavy rare earth elements (HREE)
relative to the light rare earth elements (LREE)
and slight negative Ce anomalies compared to
NASC. These data support the conclusion of Sze-
fer et al. (1999) that the REE patterns of these
sediments have not been greatly modified during
transport from their source into the southern Baltic.
The lack of significant Ce and Eu anomalies in
these plots also suggests that redox processes have
not played a significant role in modifying the
distribution of the REE in these sediments.
5.4. Inter-element relationships in view of factor
analyses data
The distribution of factor loadings for individual
elements reported here (Fig. 6b) is in good agree-
ment with dendrograms showing the patterns of
element associations in sediment samples from
Szczecin Lagoon previously obtained by Osadczuk
and Wawrzyniak-Wydrowska (1998). These auth-
ors distinguished three types of sedimentary geo-
chemical facies in Szczecin Lagoon based on
factor and cluster analysis. The geographical dis-
tribution of the facies determined by Osadczuk
and Wawrzyniak-Wydrowska (1998) (Fig. 6c) cor-
responds closely to the three main areas of the
Szczecin Lagoon identified by factor analysis in
this study (Fig. 6a). The first facies with high
contents of organic matter (OM), amorphous
SiO2 and heavy metals corresponds to the cluster
of scores with high values of F1 (Fig. 6a); the
second facies with low contents of OM, amorphous
SiO2, heavy metals and CaCO3 corresponds to the
cluster of scores with low values of F1 (Fig. 6a);
the third with intermediate concentrations of the
above mentioned constituents is transitional
between the first and second facies and corre-
sponds to the grouping of scores having values F1
of approximately zero (Fig. 6a).
As can be seen in Fig. 6b, Al is well separated
from Yb as a terrigenous normalizer. The antipa-
thetic location of these two elements mainly
reflects the element composition of the fluffy
material deposited along its transport pathways in
the lagoon (Emeis et al., 1998, 2002; Leipe et al.,
2000; Christiansen et al., 2002). The main constit-
uents of the fluffy layer are OM, Si, Al, Fe, and
varying contents of Mg and K derived principally
from minerals such as biogenic opal, quartz, mica,
clay minerals and accessory minerals (feldspar and
carbonates) (Loffler
et al., 2000). According to
Loffler et al. (2000), the concentrations of many
trace elements are correlated significantly with
particulate organic carbon and Al. Trace elements
such as Pb and Cd are preferentially associated
with clay mineral particles which form more or
less stable aggregates with OM. This results in a
significant correlation between OM, Al, Fe and
many trace elements. This conclusion is supported
by the similar distribution pattern of Al and Fe,
and trace elements such as Cd, Pb, Cu, Zn, Co,
Ni, V, Mn and Sb in Szczecin Lagoon. These
statistical results suggest that variations of the
composition of the sediments in Szczecin Lagoon
are caused, in part, by inflow of the Oder River
into the lagoon and the pattern of circulation within
the lagoon.
 G.P. Glasby et al. / Science of the Total Environment 330 (2004) 249269
6. Conclusions
Within the Polish Exclusive Economic Zone
(EEZ), Szczecin Lagoon appears to be the area
most polluted with heavy metals, especially Cd,
Zn and Pb. Sediment samples collected in October
1997 (after the exceptional flooding of the Oder
River) displayed somewhat higher concentrations
of P, Mn, Cr, Cu and possibly Cd, Pb and Zn than
those collected in December 2000. Our results
suggest that the flood resulted in the enhanced
transport of redox-sensitive and anthropogenic ele-
ments in the Oder River and their subsequent
redeposition mainly in sediments in the western
part of the lagoon. In sediment cores from the
Gdansk Basin, Cd, Pb, Zn and Cu are enriched in
upper layers of the cores but the decrease of these
elements with depth in the sediment column is not
systematic and their concentrations display maxi-
ma at certain depths within the sediment column.
The pronounced peaks of Cd, Pb, Zn, Cu and Sb
at a depth of 15 cm in core P-110 could correspond
to the presence of a sulfide-rich horizon. It is also
suggested that biogenic particles and redox proc-
esses are responsible for the deposition of Mo and
U in the Gdansk Basin, while the concentration of
V seems to be mainly controlled by scavenging
by terrigenous andyor biogenic suspended matter
during transport through the Baltic Sea.
NASC-normalised REE distribution patterns in
sediments from the study areas demonstrate that
the REE have not been greatly modified during
transport from their source into the southern Baltic.
The lack of significant anomalies for the redox
sensitive elements such as Ce and Eu implies that
redox processes have not played a major role in
modifying the distribution of the REE in these
sediments.
Factor analysis shows that Szczecin Lagoon can
be divided into three main geographical regions
corresponding to the chemical composition of the
sediments there. Based on complex analysis of
indices such as enrichment factors (EFs), correla-
tion coefficients and the distribution patterns of
factor scores, it is concluded that clay minerals
and organic material aggregate to form flocs,
which effectively concentrate heavy metals. This
fluffy material is mainly responsible for the
267
transport, deposition and enrichment of heavy
metals in the western part of Szczecin Lagoon.
Acknowledgments
This work was supported by the awards of a
NATO Collaborative Linkage Grant EST.CLG
975811 and an EU grant HPRI-CT-1999-00008 to
Prof. K.V. Ragnarsdottir and Prof. B.J. Wood who
enabled J.G. to analyze the samples in this work
by ICP-MS and XRF at the EU Large Scale
Geochemical Facility at the University of Bristol
(Access to Research Infrastructures of the EC
Improving Human Potential Programme). Richard
Brooker, Chung Choi and Tony Kemp are thanked
for their invaluable assistance with the analyses
and Dr John Dalton for organizing J.G.s stay in
Bristol. We thank Dr A. Osadczuk and Dr B.
Wawrzyniak-Wydrowska for permission to repro-
duce Fig. 6c.
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