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Marine Geology, 111 (1993) 231-244 231

Elsevier Science Publishers B.V., Amsterdam

Sediment transport pathways in the Skagerrak and Kattegat as


indicated by sediment Chernobyl radioactivity and heavy
metal concentrations

A . K u i j p e r s a, B. D e n n e g ~ r d b, Y . A l b i n s s o n c a n d A . J e n s e n d
aGeological Survey of Denmark, Thoravej 8, DK-2400 Copenhagen NV, Denmark
bDepartment of Marine Geology, Giiteborg University, Box 7064, S-402 32 G6teborg, Sweden
CDepartment of Nuclear Chemistry, Chalmers University of Technology, S-412 96 Giiteborg, Sweden
dDanish Hydraulic Institute, Agern Allee 5, DK-2970 Horsholm, Denmark
(Received May 23, 1991; revision accepted February 19, 1992)

ABSTRACT

Kuijpers, A., Denneg~rd, B., Albinsson, Y. and Jensen, A., 1993. Sediment transport pathways in the Skagerrak and Kattegat
as indicated by sediment Chernobyl radioactivity and heavy metal concentrations. In: G. Liebezeit, T.C.E. van Weering and
J. Rumohr (Editors), Holocene Sedimentation in the Skagerrak. Mar. Geol., 111: 231-244.

The concentration of the heavy metals Hg, Cu, Pb and Zn as well as Chernobyl Cs-137 radioactivity was determined in
surface sediments from the Skagerrak and Kanegat. Sediment samples from adjacent Swedish fiords were analysed as well.
The sampling was carried out between spring 1988 and autumn 1990.
Highest concentrations of heavy metals and largest Cs-137 activities occur in fine-grained organic-rich (> 2% Cot,) sediment
from Swedish inshore waters and locally also in the Kattegat. Regional trends of relative enrichment of the various heavy
metals and Chernobyl Cs-137 with respect to organic carbon was used to determine transport patterns of material enriched
with respective elements.
It can be proven that deposition of fine-grained material transported from the (southern) North Sea by the Jutland Current
is the main mechanism determining the regional accumulation of lead and Chernobyl-derived Cs-137. This mechanism princi-
pally controlls the areal distribution of mercury-enriched material as well, but it is regionally of less importance as far as the
accumulation of Cu and Zn concerns. The Chernobyl Cs-137 data show that a large proportion of the fine-grained material
transported by the Jutland Current originally is river-borne suspension load from (central) western Europe.
The areal enrichment pattern of copper, and on a smaller scale those of mercury and zinc too, points to westerly directed
suspension load transport across the Kattegat. Material enriched with these elements apparently is being discharged from
Swedish industrial and urban centers, in particular the G6teborg area.

Introduction in the western S k a g e r r a k ( N o l t i n g a n d Eisma,


1988). P a r t i c u l a r l y t h a t p a r t o f the s u s p e n d e d
T h e S k a g e r r a k a n d n o r t h e r n K a t t e g a t a r e a is m a t t e r o r i g i n a t i n g f r o m river-discharge in the
well k n o w n as one o f the few sites where a s o u t h e r n N o r t h Sea c a n be a s s u m e d to be c o n t a m i -
significant a c c u m u l a t i o n o f s u s p e n d e d m a t t e r f r o m n a t e d b y a wide r a n g e o f p o l l u t a n t s . B a n a t et al.
the N o r t h Sea occurs (e.g. E i s m a a n d K a l f , 1987). (1972) have r e p o r t e d e n r i c h m e n t levels o f n o r t h -
A s t u d y o f the e l e m e n t a r y c o m p o s i t i o n o f sus- west E u r o p e a n rivers to have reached a f a c t o r o f
p e n d e d p a r t i c u l a t e m a t t e r in the N o r t h Sea shows 5 - 1 0 0 for the h e a v y m e t a l s c o p p e r , zinc, lead,
t h a t the influence f r o m the s o u t h e r n N o r t h Sea on c a d m i u m a n d m e r c u r y . O b s e r v a t i o n s m a d e in the
the c h a r a c t e r o f the s u s p e n d e d m a t t e r is strongest D a n i s h sector o f the N o r t h Sea between 1979 a n d
1983 indicate a S - N g r a d i e n t o f the seawater
Correspondence to: A. Kuijpers, Geological Survey of Den- c a d m i u m c o n c e n t r a t i o n suggestive o f a c a d m i u m
mark, Thoravej 8, DK-2400 Copenhagen NV, Denmark. source in the G e r m a n Bight (Int. N o r t h Sea Confer-

0025-3227/93/$06.00 © 1993 - - Elsevier Science Publishers B.V. All rights reserved.


232 A. KUIJPERS ET AL.

ence, 1987). Heavy metal concentrations in the of the non-tidal currents prevailing here. A
surface sediments of Skagerrak and Kattegat have summary of the regional current pattern has
previously been studied by Olausson et al. (1972). recently been given by Fonselius (1987, 1990). The
Furthermore, Pheiffer Madsen and Larsen (1986) currents are not only controlled by the local wind
demonstrate that surficial sediments of the Kat- conditions, but they are to a large degree also
tegat have been enriched by a factor 2-3 for Zn, dependent on the general atmospheric situation
Cd, Pb and by a factor 4-9 for Hg. These rates over the northeast Atlantic, North Sea and Baltic
are comparable with those measured in recent (Dietrich, 1951; Dickson, 1973).
Baltic Sea sediments (Erlenkeuser et al., 1974). Normally, low salinity water (S<20%o) from
It should be noted that for some of the elements the Baltic flows north through the Kattegat into
dealt with, as e.g. Pb, atmospheric transport may the Skagerrak ("Baltic Current"). These water
significantly contribute to large-scale spreading of masses are mainly concentrated at the surface
the element (e.g. Murozumi et al., 1969). along the Swedish coast. In the Skagerrak and
Until the beginning of the 1960s artificial Norwegian Channel upper layer outflow follows
radionuclide input into the marine environment the Norwegian coast ("Norwegian Coastal Cur-
was exclusively attributable to atmospheric nuclear rent"). On the other hand, more saline water
bomb testing. When regarding the northwest masses are transported along the Danish coast
European shelf seas, however, since that time the from the North Sea into the Skagerrak ("Jutland
main source has increasingly been the nuclear Current") and northern Kattegat (Tomczak, 1968;
energy industry, in particular reprocessing plants. Svansson, 1975; Rodhe, 1987).
In the region dealt with, one nuclear energy station As illustrated in Fig. 2, the actual hydrographic
(Ringhals) is located on the Swedish coast border- conditions can, however, strongly differ from the
ing the Kattegat. Analysis of sediment sampled general pattern outlined above. This figure shows
from the surroundings of Ringhals in 1984 a situation of marked salinity gradients in the
revealed, however, that most of the Cs-137 radioac- northern Kattegat which results from strong
tivity originated from the UK reprocessing plant outflow of springtime (melt)water from amongst
Sellafield (Notter, 1986). This is attributable to others, the G6ta River (G6teborg area) into the
the current system prevailing in the North Sea, Kattegat.
which favours the transport of radionuclides from According to Eisma and Kalf (1987), about 40
the reprocessing plants in the UK (Sellafield) and million tons (dry weight) of suspended matter is
France (La Hague) towards Skagerrak and Kat- transported through the North Sea annually. Half
tegat (Kautsky, 1985). A more recent input of the amount is concluded to originate primarily
artificial radionuclides is due to the nuclear from sources in the southern North Sea. These
accident at Chernobyl in 1986, with fallout having authors estimate that 50-70% of the suspended
been particularly severe in the Baltic region (e.g. matter is deposited in the Kattegat-Skagerrak-
Nies and Wedekind, 1987). Norwegian Channel.
Aim of the present study is to determine the Van Weering et al. (1987) indicate a comparable
areal enrichment patterns of selected heavy metals amount of sediment to accumulate annually in
and radionuclides in surface sediments, in order the Skagerrak. Previously, Rodhe (1973) calculated
to reveal sediment transport pathways and to link that the amount of suspended matter entering the
these to the regional hydrography. Figure 1 shows eastern Skagerrak and Kattegat is in the order of
the location of the study area with the sampling 8 × 10 6 t/yr. Also other observations (Van Weering,
stations. 1981; F/ilt, 1982) point to a significant sediment
transport from the Skagerrak into the northern
Hydrography and recent sedimentation Kattegat.
In the Skagerrak fine-grained silty and muddy
An important characteristic of the hydrography sediments are deposited only at water depths in
of the Skagerrak and Kattegat is the variability excess of about 70 m. As previously shown by
SEDIMENT TRANSPORT PATHWAYSIN THE SKAGERRAK AND KATTEGAT 233

12 °
+%° + STROMSTAD +

NORWAY .'-
:" V7~
• -, %w
SWEDEN

+ 5 8 °

• :. " ... 7~1"2~ #5 ..:: "~4 ~7 2625


. . . . . . jTo. -,103 - . 7 , _ #2:#9 ca" p
I GOTEBORG
~oI ~ 05
.lo6

/
'

FREDERIKSHAVN
l
~319 .12"_
: 8 ~ 7' ~4

........
,,
~..'..
,i •
i ~

j6 ~5~1 pl
~1 ~ p

/
/
J
/ / ~ _

~I ~2 ?6

DENMARK

,st-t ....
W "~
\ I+

10 °
+ I 5¢]
Fig. I. Location of the sampling stations with the main features of the regional bathymetry.

Van Weering (1981), the sediment organic carbon records (Van Weering, 1981; Denneg~%rd and
content in this area is well associated with the Liljestrand, 1988).
clay-size fraction. In the northern Kattegat a
significant mud accumulation area is located on Methods
the western slope of the "Djupa R/innan" (Ffilt,
1982). This is the channel running along the Sediment sampling was carried out with RV
Swedish coast in the northern Kattegat (Fig. 1). Svanic, G6teborg University, between April 1988
Pb-210 measurements indicate very high sediment and August 1990. Positioning was by the Decca
accumulation rates of up to 10mm/yr on the navigation system.
slope of the channel (Jensen, 1980). Another area Sediment samples were obtained using a 10 m
of high sediment accumulation rates in excess of piston corer, a 1 m gravity corer and a box corer
4 mm/yr is found in the northeastern Skagerrak (0.3 x 0.3 x 0.5 m). Only samples obtained by box
(Van Weering et al., 1987). The fine-grained corer and gravity corer are referred to in the
sediments in these areas commonly are observed present study.
to have a high gas content displayed on seismic After onboard description of the surface sedi-
234 A. KUIJPERS ET AL.

was applied for all elements except for Zn (flame).


For mercury, 4 g of sediment was treated with
Aqua Regia (Olausson, 1975) and extracts were
~S z~/322 analysed with a flameless mercury analyser (Per-
kin-Elmer Coleman MAS-50).
Artificial radionuclides Cs-134 and Cs-137 were
measured by gamma-spectroscopy at the Danish
Isotope Centre in Copenhagen and at the Institute
of Nuclear Chemistry of Chalmers University of
Technology in Grteborg. Dry samples of 250 ml
were counted for 24 hours with a Ge (Li) detector.
A Quaternary clay from a quarry was used as
calibration standard. The clay was dried and
pulverized. 250 ml was checked for an eventually
original content of Cs-137. The efficiency of the
,,r~/ , / / l i e ~,o
Ge (Li) detector obtained from this standard was
15% and the same efficiency was assumed for Cs-
l IA,)_. 134. Detection limit for Cs-137 was 2 Bq/kg and
for Cs-134 0.5 Bq/kg.
The Cs-137 contribution from Chernobyl was
calculated from the Cs-134 activity assuming a
Cs-134/Cs-137 activity ratio of 0.55 on April 26,
Fig. 2. Surface water salinity in Skagerrak and Kattegat, April
1986. It was further assumed that the short-lived
1987 (Fonselius, 1990). isotope Cs-134 (T1/2 of about 2 yrs) originates
entirely from the Chernobyl fallout.
For sample standardization, ratios of respective
ment, 2 subcores were taken from the box core. elements to organic carbon have been calculated.
Additionally, separate samples were obtained from For each element, the minimum value of this ratio
the 0-2cm and 10-12cm depth interval. These has been defined to be the reference for the other
samples were stored at low temperature in 100 ml samples to compare with. This was done in order
plastic vials and analysed in the laboratory for to illustrate the areal enrichment pattern of
Corg, N and the heavy metal content (Hg, Pb, Cd, respective element with respect to organic carbon.
Cu, Cr, Ni, Zn). At a number of sites duplicate As for Cs-137 activities known to be mainly
box cores were collected in order to obtain large- associated with the clay mineral content, this
quantity (1 kg dry weight) samples for radionuclide standardization method will be discussed in more
analysis. Before measuring the Cot,, N and heavy detail later in this paper.
metal content, the subsamples were freeze-dried In order to reduce effects of local patchiness
and homogenized. After removal of inorganic induced by individual stations, a statistical kriging
carbon (Hedges and Stern, 1983), the sediment treatment using a weighted-moving-average inter-
organic carbon and nitrogen content was deter- polation method has been applied to the analytical
mined with a Carlo Erba NA 1500 C/N analyser. data set (Nyborg et al., in prep.). The results thus
For the heavy metals Pb, Cd, Cu, Cr, Ni and obtained have formed the basis for a block grid
Zn, 1 g of sediment was used and treated with for establishing the isoline patterns.
7 M HNO3.
After filtration, the concentration of various Results
elements in solution was measured with a Perkin-
Elmer 5000 atomic absorption spectrophotometer. For the present study a selection has been made
A graphite furnace atomic absorption technique from the total number of elements analysed. The
SEDIMENT TRANSPORT PATHWAYS IN THE SKAGERRAK AND KATTEGAT 235

selected elements are Hg, Cu, Pb and Zn as well 859 ng/g Hg measured at station 62. High concen-
as the Cs-137 contribution from the Chernobyl trations locally also oCcur in the northern Kattegat
accident. Only the surface 0 - 2 c m sediment (station 21) and in the northern entrance of the
interval is dealt with. Geographical positions of Sound at station 101. Notably low values, i.e.
the stations are referred to on Table 1. below the detection limit ( = 1 0 n g / g H g ) were
Sediment sampled is predominantly bioturbated measured in the southern Skagerrak at stations
silty clay and clayey silt. Sediment surface colors 102 and 108. In addition, station 107 yielded a
are generally light olive grey (5Y5/2) or moderate low concentration of only 17 ng/g Hg.
olive brown (5Y4/4). Below a thin (1-2cm)
oxidized surface layer colors turn to mainly (dark) Copper (Fig. 5)
grey indicative of sub- and anoxic conditions. Copper also had the highest concentration
Sediments collected off the Danish coast in the (40 Ixg/g Cu) at station 62 near G6teborg. High
Kattegat and in the southern part of the Skagerrak concentrations were locally found also elsewhere
are generally coarser and consist of sand. In these in the Swedish fjords as well as at stations 77 and
sediments the boundary between the oxidized 79 in the southeastern Kattegat. Copper concen-
surficial sediment la~/er and non-oxic sediment trations are low in sandy sediments from the
below is commonly found at greater depth southern Skagerrak. A minimum concentration of
(> 2 cm). Sand and coarser debris was found at 0.9 mg/kg Cu was measured in sediment from
station 16, northeast of Laes6. station 102.
For each individual station the sediment organic
carbon content, the concentration of the heavy
Lead (Fig. 6)
metals and the Chernobyl Cs-137 specific activity
The highest concentration (37 ~tg/g Pb) was
is given in Table 1. In contrast to the results
found in sediment from station 77 in the Kattegat,
presented for organic carbon and heavy metals,
with another peak value measured in sediment
not all stations have been analysed for Cs-137.
from nearby station 79. At inshore station 71 a
Data given here are from stations with numbers
nearly similarly high concentration was found.
between 7 and 84.
Low concentrations are typical of the sandy
Figure 3 shows the areal distribution of the
sediments present in the southern Skagerrak,
organic carbon content in the upper 2 cm of
sediment. It should be borne in mind that Figs. 4 where station 102 yielded a minimum of 2 ~tg/g
to 8 show the results from statistical kriging Pb.
treatment of the heavy metal and radionuclide
data. Analytical results for respective elements are Zinc (Fig. 7)
summarized in the following. The highest zinc concentrations occur in the
Swedish fjords with a maximum of 190 I~g/g Zn
Organic carbon (Fig. 3) measured at station 72. However, high concen-
The highest values in excess of 3% Co~g were tration levels were also found off the Swedish
measured at the stations 76, 77 and 78 in the coast, in particular in the southeastern Kattegat
south eastern Kattegat. Such high values locally (stations 77 and 79). The zinc concentration is
also occur in Swedish inshore waters near G6teb- low in the southern Skagerrak, where a minimum
org (stations 62 and 64). A low organic carbon of 0.9 I~g/g Zn was measured in sediment from
content (< 1.0%) is typical of the sandy sediments station 102.
sampled in the southern Skagerrak. A minimum
value of 0.05% Corg was found here at station Chernobyl Cs-137 (Fig. 8)
102. Sediments from the Swedish fjords appear to
have the highest specific activity, with a maximum
Mercury (Fig. 4) of 46 Bq/kg (dry weight) Chernobyl-derived Cs-
Sediment sampled near G6teborg contains the 137 occurring at station 62 located near G6teborg.
largest amount of mercury with a maximum of Another relatively high value (32.5 Bq/kg) was,
236 A. KUIJPERSET AL

TABLE I

Sampling position, water depth and sediment content of Corg, Cs-134 and
Cs-137 (Chernobyl), Hg, Pb, Zn and Cu
l.ongitude Latitude D~th Corg Ca - 137 C s - 134 Hg lab Zn Cu
E N m % (Chemobyl) Bq~g ng/g p /g ~l/g p~g
BqJkg
01 11.3950 57,2963 33 229 050 250 1~40 130
02 t 1. 3525 57, 27 40 ~)2 1 95 96 0 21 0 103 0 12 0
03 I 1, 31.36 572620 68 212 280 220 930 110
04 11,2581 57,2520 74 195 1610 200 910 120
05 11.2887 57,24 I1 82 209 1590 2~0 970 120
O6 1 I, 24 62 57, 23 79 67 2 18 80 0 230 106 0 ~3 0
07 1 I, 37.46 67.24 09 61 2 18 80 0 23 0 103 0 13 0
K81 I I, 2987 67.26 34 67 18 0 1480 190 88 0 11 0
09 11,5618 " 87,1.518 46 254 350 280 1240 1.50
10 11.5~ 66 87, 07 04 ~5 272 31 0 270 141 0 16 0
11 1 I, 54 44 57, o3 07 49 226 8o0 21 0 I090 13 0
12 11,08 06 67.32.92 40 1 81 140 0 20 0 820 12 0
~3 11,1987 57.34 40 49 1.59 75.0 190 83.0 120
14 11.25,40 37, 36.50 74 1.75 140 80 108.0 23.0 970 120
15 11 2736 87, 50.50 50 166 106 60 910 18.0 770 110
17 10.61 80 57.28.07 37 1.98 148.0 230 93,0 130
16 10.45.52 $7, 25.88 29 182 104 69 99.0 190 660 120
I~ 10158.70 57.32..31 33 1.62 1420 180 720 100
20 11, 02.50 57.3O.39 31 1.24 7.2 41 93.0 150 60.0 90
21 11.05.85 67.40,86 33 1.07 3920 14.0 60.0 10 0
22 1 I. 13.41 57, 3081 40 157 93 53 1250 19.0 78.0 10.0
23 11, 24.43 57, 4033 96 203 21.0 24.0 89.0 11 0
24 11.1810 57, 46.22 62 1.67 7.3 43 115.0 E2.0 70.0 110
25 11,13.40 57. 3343 72 171 14.6 83 12~0 21 0 81.0 110
26 1 I, 04.17 57.54.23 72 15 0 10 0 82 480 13.0 47.0 80
27 10, 5470 57, 6232 93 990 74 0 120 37 0 5.0
28 10.48.50 67, 40.73 90 580 430 90 25.0 4.0
29 I 0. 44.32 57, 4402 22 630 8I 36 46 0 70 -- 40
30 10,47 73 87.3(.49 -- -- 44 25 . . . .
31 11, 26.03 57.28.53 50 1 29 930 170 630 90
32 10.29.74 58, 50.03 110 166 1050 190 830 100
33 10. 29.04 37.37.16 100 1.83 840 220 800 100
3~ 10.39.21 67.67 23 150 2.50 80.0 ~20 87.0 12.0
10.45.03 87.58.14 180 208 119.0 L:~0 98.0 12.0
36 11, 03.83 50. 08.08 140 18 2 1060 200 830 100
37 10.83.10 58. 05.58 190 223 1060 240 99.0 130
38 10. 49.01 58, 92.38 200 226 76.0 26.0 07.0 14.0
39 I0, 05.98 58, 50.11 140 143 1090 17.0 68.0 100
4O 1 I, O3.32. 05, 03.31 13O I 68 78.0 21.0 80.0 100
41 11, 07.30 57, 59.66 87 175 98.0 21,0 77.0 10.0
42 10.50,43 67. 3g.M; 29 124 9O0 15.6 67,6 08
43 10.81.92 67. 33.90 27 1.50 1042 15.8 54,2 76
44~ I 1.01.35 57, 27.84 30 0.99 124 7.1 644 10.3 334 43
11,3131 57, 30.50 60 226 150.2 34.0 110.0 175
44~ 11, 1880 67, 41.04 49 163 141.8 24.9 84.0 128
11.21 10 57, 44.§7 95 2.12 1890 290 950 161
48 11, 21,02 67, 49.82 66 187 179+6 28.4 86.8 12 0
40 11.39.00 67, 26,11 19 048 39.5 89 Z2.8 31
50 11.37.10 57.36.57 16 0.84 12.2 89 57.0 92 331 40
51 10, 6;~.50 67.50,61 93 0.72 771 44 5451 101 31.3 38
82 10.14.50 57, 50.03 78 110 111 83 920 14 2 45.2 63
63 I0, 01.50 67, 51 09 62 123 15.o 8.6 806 160 54).3 70
54 09.52.03 57~ 58.52 99 0.32 O 0 s2.1 7.0 208 22
55 00. 41.01 87.5504 98 0.48 8.1 36 83.1 8.0 23,7 2.6
56 10.13.03 57.67.31 80 1.36 10,0 57 118,2 19.7 643 87
67 I0.15.07 58, 03.48 108 I 71 17.5 100 1294 20.1 63.1 8.7
58 10. 23.10 58, 50.01 160 165 18.4 105 1009 22.3 83.8 8.6
5(~9 11.01.20 57.445.75 41 1 11 13+8 79 103.8 15.0 50.3 7.3
11.12.81 $7. 43.59 42 13O 1369 16.8 81.0 9.3
81 11.31,50 07, 30,50 65 1.o5 504 101 5.0.8 67
82 11, 49.24 57.40.22 11 3.74 48.0 26.2 8588 23.9 15~.0 399
63 11.47.22 57. 40.54 13 1.61 125.8 10.5 75.5 16.8
84 11.41.39 67,40.31 21 3.24 20.8 17.0 375.1 26.7 119.0 25.2
65 11.43.22 57, 46.10 12 2.84 40.1 22,9 548.8 22.6 1420 24.6
66 11.44.41 37.46.44 4 2.71 44.3 25.3 2440 13.2 105.0 17.7
87 11.2t5.33 57.46.09 48 1.57 1138 18.2 73.8 11.1
68 11.10.O5 07.52.50 38 2.09 157 6.9 172.8 17.0 793 13.3
69 1 I. 18.50 57.61.11 91 1,88 193.2 222 926 16.5
70 11.24.34 67.55.25 46 L31 16.7 9.5 104)8 173 73.3 93
71 11.32,42 58. 1999 101 3.21 43.0 25.0 130.9 33.4 1560 233
72 11, 48.46 58. 1895 39 295 28.3 16 0 178.3 22.8 190.0 293
73 11, 45.38 57.5913 16 266 33.7 19.2 1913 296 143.0 243
74 12, 10.25 57, 0452 23 037 O 0 37.0 52 29.7 2.1
76 120246 57, 50.72 50 2.48 19 3 110 749 273 1200 169
78 12,1834 56,5002 32 194 237 135 370 255 1030 ~27
77 12, 39.71 56. 3282 20 389 32 5 185 58 5 36 B 134 0 203
78 12.2978 56.3313 25 330 11.0 83 514 122 519 59
78 12.2363 56, 3O.36 35 316 163 104 270 363 1420 208
80 12. 12,48 56, 3O.92 53 2 95 249 14 2 860 29 9 1300 170
81 11.53.32 56. 89.88 31 0.47 0 0 324 57 3O3 30
82 12.03.67 50.50.03 44 2.55 210 120 365 ,308 1210 18.3
~8~ 12.04.34 50, 50 53 46 0.64 105 60 444 8.9 447 52
I1, 59.22 97, 18.01 34 2.22 195 111 M9 287 1040 168
85 11.09.50 07.37.40 77 1 18 123 4 12 2 97.4 7.4
11.21 ./AS 58. 19.30 32 236 1739 25.8 118,0 16.3
11, ~*,30 50.3150 63 1.82 79.5 20.6 9411.3 12.9
88 11, 04.76 58. 3627 60 1 66 836 18 4 780 9.9
~0 10. f,2.0~ 54. 05.75 76 160 118.8 20.3 89.4 11.4
1 I. 04.24 57, S0.(~ 50 094 95.4 1t 3 54.5 6.6
01 10. 54.42 07.48.85 58 086 87.6 93 44.6 6.3
9~ 10. 46.50 37.40.89 40 057 63.9 98 35,8 4.8
11.00.12 541,~ . 1 6 93 181 1254 19.8 91.3 111
94 11,05.35 58. 50.50 109 232 95.4 27.6 118,0 16.5

10.4750 M , 40.50 215 1459 255 110.0 14.0


97 10.33 M 56.48.32 110 I 58 886 218 81.7 10.9
98 10.48.00 58,40.92 112 210 155.0 266 98.0 126
99 10.0530 58,34.30 148 168 131.3 231 840 11 1
100 12, ~0 18 50.17.33 27 173 574 182 838 11 1
101 12. ; ~ 5 0 50,10.50 24 093 3488 10.3 41 8 64
102 9, 2350 57, 44.15 32 005 O0 2.3 89 09
103 9, 0~ 93 57.47,50 129 053 465 57 30 2 40
104 8.4847 57, 48.07 192 073 37 6 92 36 6 53
105 8.4317 87, 36.09 89 042 250 54 257 30
106 8. 4250 67, 3O.04 64 032 20.5 6.9 18 5 20
107 8, 20.50 57.36.116 64 0.72 16.5 73 24 2 41
105 9.18,O3 57.41.50 266 2.48 0.0 218 794 133
109 9.88.43 $7.44 .~3 304 1.39 48.9 187 604 01
110 II. 93.18 57. 48 92 2O2 O,56 3O.0 89 ~5 3.o
111 0, 00.42 37, 01 0 5 237 10 7 28.0 10 2 34 5 82
112 9,13.91 87.53.90 210 0.70 41,0 91 350 42
113 0, 42.79 50, 03.85 311 131 43,8 11 0 469 80
I '~4 8, 5 7 11 58. 0308 165 1,50 58 5 109 462 69
115 10.3601 S~. 01 O0 180 150 1054 236 t;156 135
118 11, 30 44 57, 11 50 188 208 740 229 1020 148
SEDIMENT T R A N S P O R T PATHWAYS IN THE S K A G E R R A K A N D KATTEGAT 237

,B'sg.
NORWAY ~ *

? SWEDEN

P eo ,oo

:'i)
DENMARK'

(a) +,. ~o. T ~.

Fig. 3. The organic carbon content (%) of surface sediment


(0-2 cm) in Skagerrak and Kattegat. NORWAY ;~)
J
SWEDEN

however, measured in sediment from station 77


in the southeastern Kattegat. Levels below the
detection limit (< 2 Bq/kg) were found at station
74 and 81 in the Kattegat and at station 54 in
the Skagerrak. Generally, sandy sediments in the
southern Skagerrak and northern Kattegat have
a Chernobyl Cs-137 contribution of less than
15 Bq/kg (dry weight). Within this context it is "+.

worthwhile mentioning that Cs-134 specific activi- DENMARK


ties measured were generally between 2.5 and m
9.0 Bq/kg (dry weight; Kuijpers et al., 1989). With
the exception of one station (27), the Cs-137
Hg/Co~
contribution from other sources (e.g. Sellafield)
{b)
clearly exceeded the Chernobyl-derived Cs-137
specific activity by a factor of up to 2.5 at the
Fig. 4. (a) Sediment mercury concentrations (ng/g Hg) in the
maximum. upper 0-2 cm of sediment. The isoline patterns in Fig. 4a and
b have been obtained from statistical kriging treatment of the
Discussion analytical data set. (b) Relative enrichment of mercury with
respect to organic carbon in comparison with the reference
sample (108). Arrows indicate transport pathways of mercury-
Studies on h e a v y m e t a l c o n c e n t r a t i o n s in the enriched material.
surficial s e d i m e n t s o f S k a g e r r a k , K a t t e g a t a n d
a d j a c e n t Swedish fiords were p r e v i o u s l y p u b l i s h e d
b y O l a u s s o n et al. (1972), P e d e r s t a d et al. (1980),
238 A. KUIJPERSET AL.

Fig. 5. (a) Sediment copper concentrations (~tg/gCu) in the Fig. 6. (a) Sediment lead concentrations (~tg/g Pb) in the upper
upper 0-2 cm of sediment. The isoline patterns in Fig. 5a and 0-2 cm of sediment. The isoline patterns in Fig. 6a and b have
b have been obtained from statistical kriging treatment of the been obtained from statistical kriging treatment of the
analytical data set. (b) Relative enrichment of copper with analytical data set. (b) Relative enrichment of lead with respect
respect to organic carbon in comparison with the reference to organic carbon in comparison with the reference sample
sample (78). Arrows indicate transport pathways of copper- (78). Arrows indicate transport pathways of lead-enriched
enriched material. material.
SEDIMENT TRANSPORT PATHWAYS IN THE SKAGERRAK AND KATTEGAT 239

~" , SWEDEN
/ is

• se° ~o.~ " : " " "

l/'!.'a' /
NORWAY ~ ~
SWEDEN

+ +, *~7

DENMARK

r
Cso137/C~
(b) ~ ~° 1 \

Fig. 8. (a) Chernobyl-derived specific activity of Cs-137 (Bq/


Fig. 7. (a) Sediment zinc concentrations (ktg/g Zn) in the upper kg dry weight) in the upper 0-2 cm of sediment. The isoline
0-2 cm of sediment. The isoline patterns in Fig. 7a and b have patterns in Fig. 8a and b have been obtained from statistical
been obtained from statistical kriging treatment of the kriging treatment of the analytical data set. (b) Relative
analytical data set. (b) Relative enrichment of zinc with respect enrichment of Chernobyl Cs-137 with respect to organic
to organic carbon in comparison with the reference sample carbon in comparison with the reference sample (24). The
(78). Arrows indicate transport pathways of zinc-enriched arrow indicates the transport pathway of cesium-enriched
material. material.
240 A. KUIJPERS ET AL.

Lyngby and Brix (1984) and Cato (1977, 1986, activity measured in suspended matter collected
1990). from the coastal zone of the German Bight in
The surface sediment concentrations of the December 1986 still yielded high values of up to
elements Cu, Pb and Zn found in the present 150 Bq/kg Cs-137. In the Baltic it was found that
study are clearly higher than those reported by more than one year after the Chernobyl accident
Olausson et al. (1972). For the element Hg Cs-137 activities started to increase in the southern
concentration levels are about the same. Zinc parts. This can be ascribed to water mass transport
concentrations measured in surface sediments from from the Aaland region initially most severely
the Skagerrak in the late 1970s (Pederstad et al., affected by Chernobyl fallout. Chernobyl-derived
1980) have comparable or slightly higher values Cs-137 specific activities measured in fine-grained
than those published by Olausson et al. (1972). sediments from the Bay of Lubeck, southwestern
The concentrations of Cu and Zn in near-shore Baltic, reached maximum values of up to 200 Bq/
sediments between Skagen and Frederikshavn kg. Sediment from the German Bight had specific
(Lyngby and Brix, 1984) are comparable or slightly activities of up to 20 Bq/kg Cs-137.
lower than the concentrations found in the present The Chernobyl contamination of the sites inves-
study for stations further offshore. The heavy tigated in the Baltic and North Sea did not reach
metal concentrations from stations in the Swedish further down than 5 cm subbottom depth one
fjords as given in the present study are comparable year after the accident (Nies and Wedekind, 1987).
with those reported from that area by other Interestingly, Cs-137 analysis of surface sediment
authors (Cato, 1977, 1986, 1990; Bornmalm, 1987). from our stations 54, 74 and 81 revealed virtually
The Cs-137 sediment contamination induced by no Chernobyl radioactivity, whereas at another
the Chernobyl accident can be stated to reach a station (24) a Chernobyl Cs-137 peak was found
level comparable to that induced by Sellafield at 10-12cm subbottom depth instead of at the
peak discharges in the period 1974-1980. Sediment surface (see Kuijpers et al., 1989). In addition, at
sampled in 1984 from the surroundings of Ringh- station 29 near Skagen the Chernobyl Cs-137
als, eastern Kattegat, yielded up to 66 Bq/kg (dry radioactivity was the same at 0-2cm and at
weight) Cs-137, which for the largest part was 10-12 cm subbottom depth. At all other stations
ascribed to Sellafield discharges (Notter, 1986). the Chernobyl Cs-137 peak occurs in the topmost
Within this context it should be borne in mind few centimeters of the sediment column, with a
that our sediment sampling started two years after minor Chernobyl Cs-137 activity detectible at
the Chernobyl accident. Kautsky et al. (1980) and 10-12 cm depth. This can be attributed to biologi-
Kautsky (1985) indicate a transport time for cal mixing which may affect the sediments down
waters from the German Bight, North Sea, to to 22 cm subbottom depth (Jensen, 1980). With a
reach the northern Kattegat of about one year. A sediment accumulation rate not exceeding l0 mm/
direct Chernobyl Cs-137 fallout in the Skagerrak yr (Jensen, 1980; Van Weering et al., 1987), it
region could be proven by the study of sediment must be evident that a lack of Chernobyl radioac-
trap samples collected immediately after the acci- tivity at the sites mentioned has to be ascribed to
dent (Kempe and Nies, 1987). However, Nies and mechanical reworking as induced by current- and
Wedekind (1987) were able to show that in May wave-action, trawling etc.
and June 1986 radionuclides from Chernobyl A presentation of absolute heavy metal concen-
fallout were most dominant in the coastal zone trations and radioactivity values only without a
of the southeastern North Sea and Skagerrak, standardization for various sediment types
whereas elsewhere in the North Sea artificial sampled would not provide us with further
radioactivity had to be ascribed mainly to Sellafield indications on sediment distribution pathways.
contamination. These authors also demonstrated From many studies it is known that fine-grained
that North Sea water radioactive contamination sediments generally have a higher organic carbon
from Chernobyl was persistingly significant off the content. Moreover, it could be illustrated that
Elbe estuary until late summer 1986. The Cs-137 heavy metal concentrations well correlate with the
SEDIMENT TRANSPORT PATHWAYS IN THE SKAGERRAK AND KATTEGAT 241

sediment organic carbon content (e.g. Kuijpers, heavy metals and radionuclides are the clay
1974; Cato, 1977, 1986; Abu-Hilal and Badran, mineral composition and sediment redox con-
1990). Hamilton (1989) reports that also radionu- ditions.
clides are preferably associated with organic-rich Clay mineralogical analysis of recent surface
material. Other evidence (e.g. Wilken and Diehl, sediments from the Danish sector of the Skagerrak
1989), however, indicates that Cs-137 is mainly and from the central northern Kattegat has
bound to clay minerals, in particular to illite. revealed virtually no compositional differences to
Van Weering (1981) showed that the sediment occur in this area (Pederstad et al., 1980; Wirth
organic carbon content in the Skagerrak is well and Wiesner, 1988). This implies that the amount
associated with the clay fraction in the well-sorted of illite does not vary much either, which may
sand to moderately-sorted silt population. Further- permit a standardization also of Cs-137 to Corg
more, Wirth and Wiesner (1988) demonstrated which likewise only little fluctuates in the < 20 ~tm
that the total organic carbon content in the fraction.
<20 txm fraction of surface sediments in the The other relevant factor thus to consider is
Skagerrak does not display any significant regional the sediment redox condition. Not regarding the
change. Thus, regardless of the sediment type, a boxcores taken in the Swedish fjords, our surface
well-defined relationship appears to exist between sediment samples can be concluded to have all
organic matter content and the finest fraction of been taken from above the oxic-anoxic sediment
our sediment sampled, including the clay mineral interface. This is concluded from the appearance
content. of precipitated black FeS in the darkgrey non-
Grain-size fractionation in the laboratory has oxic sediments below. It is evident, however, that
been proven to yield major uncertainties with the oxidized surface layer is thicker (>>2 cm) in
regard to trace metal contents. This can be the sandy sediments off northern Denmark than
ascribed to cluster formation during drying (see elsewhere in the area. More detailed studies on
also Stevens, 1987), inducing an anomalously high surface sediment redox conditions in the Skagerrak
metal content in medium and coarse sediment and northern Kattegat have been made by, e.g.,
fractions (Krumgalz, 1989). Also Lohse (1988) Fossing (1991).
reported that such a fractionation was less useful Summarizing, relative enrichment trends of the
when compared with a standardization based on heavy metals and Cs-137 with respect to organic
total organic matter. By using the organic carbon carbon are not likely attributable to regional
content, Knickmeyer and Steinhart (1988) and changes of the sediment grain size, the clay
Cato (1977, 1986, 1989) revealed the geographic mineralogy or the sediment redox conditions.
differences in sediment organochlorine and heavy Thus we may conclude that Figs. 4b-8b indeed
metal contamination, respectively. However, other show regional transport pathways indicative of
relevant factors are to be taken into consideration sources that are specific for respective elements.
as well. Figure 4b illustrates the discharge of mercury-
A major regional change in the composition of loaded material from the GSteborg area. This
the organic matter could influence the sorption material apparently spreads in west-northwestern
potential of heavy metals and radionuclides. direction where part of it is deposited. The figure
Wiesner et al. (1990) reported that 50-70% of the further indicates that transport of material from
total organic matter in recent sediment of the the North Sea into the northern Kattegat also
Skagerrak is terrestrial in origin. These authors contributes to mercury accumulation in the area.
further state that increases in the total organic In case of copper (Fig. 5b), it is evident that
matter content are coupled with an increase of discharge of copper-enriched material from the
both marine and terrigenous inputs. We may thus Grteborg area controlls the copper accumulation
assume that organic matter sorption characteristics in the sediments of the Kattegat north of Laes6.
are not much differing throughout the Skagerrak. A secondary input of minor importance from the
Further factors controlling the enrichment of North Sea is confined to the southwestern Skager-
242 A. KUIJPERS ET AL.

rak. Figure 6b clearly illustrates the flux of lead- that of mercury and zinc, in Kattegat sediments
enriched material from the North Sea into the seems from a hydrographical point of view more
Skagerrak and northern Kattegat. A secondary problematic. The presence of a deep channel
minor and local source can be allocated in the parallel to the Swedish coast and the occurrence
eastern Kattegat (Varberg area). Moreover, a of intermittent bidirectional currents along the
major input of zinc-loaded material can also be Swedish coast would certainly not suggest the
allocated in the Varberg area (Fig. 7b). Other patterns observed. A mechanism enabling the
inputs of zinc are the inflow of zinc-enriched transport of, for example, copper-enriched mate-
material from the North Sea into the Skagerrak, rial across the deep channel to the central Kattegat
and a more local discharge into the eastern north of Laes6 can only be provided by suspension
Skagerrak from the Uddevalla area. The Cherno- load transport. Within this context we may refer
byl Cs-137 contamination of surface sediments in to Fig. 2 which illustrates the salinity distribution
the Skagerrak and northern Kattegat unambigu- in surface waters of the Kattegat and Skagerrak
ously originates from input of fine-grained material in April 1987. These hydrographic conditions
from (southern) North Sea origin (Fig. 8b). recorded after a severe winter show large-scale
The transport of suspended matter and contami- meltwater discharge from the Grta river (Grteb-
nants from the southern North Sea into the org) area, which affects the hydrography of the
Skagerrak and northern Kattegat is known from entire Kattegat north of Laesr. Thus we have
many studies (Eisma and Kalf, 1987; Knickmeyer evidence that suspension load transport from the
and Steinhart, 1988; Lohse, 1988). In case of the Grteborg area as proposed above could occur,
Chernobyl Cs-137 contamination, however, the and is probably most effective in early springtime
well-defined enrichment trend as shown in Fig. 8b when meltwater discharge is largest. Flocculation
was not to be expected, as the Swedish mainland processes generally activated at strong salinity
and Baltic region were much more affected by gradients (see Fig. 2) may favour the deposition
fallout than the North Sea (see also above). To of part of this fine-grained material discharged
explain the pattern found we conclude that the from the Swedish mainland.
Chernobyl radioactivity in the Skagerrak and
northern Kattegat must originate from deposition Conclusions
of contaminated river-borne (e.g. Rhine, Elbe)
suspension load from central western Europe, The highest concentrations of the heavy metals
where fallout was severe as well. Hg, Cu, Pb and Zn occur in fine-grained organic-
Local discharges from Swedish industrial and rich ( > 2 % Cor~) sediments from the Swedish
urban centres also significantly contribute to the t]ords and at some sites in the Kattegat. The
regional heavy metal (Cu, Zn) accumulation. Zinc concentration of these heavy metals is generally
is known to be the main heavy metal in both low in the sandy sediments from the southern
Swedish industrial and urban waste water dis- Skagerrak. Also the Chernobyl contribution of
charged into the Kattegat and Skagerrak (Thorell, Cs-137 activity was found to reach peak values in
1980). Copper and its alloys, as amongst others Swedish inshore waters and at a site in the
bronze etc., has many applications in such indu- southeastern Kattegat.
stries as shipyards and other steel industries After standardization based on the total organic
present in the Grteborg area. The element copper carbon content, we conclude with the help of
occurs in the aquatic environment mainly as a statistical analysis from the areal enrichment
complex with dissolved and colloidal organic trends of various elements with respect to organic
matter and is further mostly associated with carbon the following:
suspended particles (Donze et al., 1990). On a regional scale, input of material from the
In contrast to distribution patterns attributable (southern) North Sea by the Jutland Current is
to Jutland Current transport, the explanation of the main mechanism determining the accumulation
the copper enrichment, and to some extent also of lead and Chernobyl-derived Cs-137. This mech-
SEDIMENT TRANSPORT PATHWAYS IN THE SKAGERRAK AND KATTEGAT 243

anism is also important when regarding the References


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