Environmental Pollution, Vol. 92, No. 1, pp. 73-78, 1996
Copyright © 1996 Elsevier Science Ltd
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ELSEVIER
SPATIAL A N D TEMPORAL VARIATIONS OF TRACE METALS
IN BOTTOM SEDIMENTS OF PETER THE GREAT BAY, THE
SEA OF JAPAN
A. V. Tkalin, a B. J. Presley, b* & P. N. B o o t h e b
aFar Eastern Regional Hydrometeorological Research Institute (FERHRI), Vladivostok 690600, Russia
bDepartment of Oceanography, Texas A&M University, College Station TX 77843-3146, USA
(Received 18 May 1995; accepted 7 September 1995)
STUDY AREA
Abstract
New data on trace metal distribution in bottom sediments
o f Peter the Great Bay (the Sea of Japan) are presented.
Much higher concentrations were detected near the most
likely anthropogenic sources o f trace metal inputs (waste
water discharges from Vladivostok and Nakhodka, and
the Vladivostok coastal ltmdfill). Sediments in these contaminated areas were up to 700 ppm in Zn, 530 ppm in
Pb, 7 ppm in Cd and 3 ppm in Hg. River runoff is of
minor importance as a metal source in the investigated
areas. The spatial distribution of trace metals outside the
areas directly influenced by sewage discharges is regulated by natural processes such as sediment sorting by
grain size. Based on radiometric dating of sediment cores,
increases in the trace metal content of bottom sediments
near Vladivostok begun in approximately 1945.
Bottom sediment samples were collected in September-October 1994 in the Peter the Great Bay area of the Sea
of Japan (Fig. 1). More specifically, the following areas
were sampled:
• The inner harbor of Vladivostok, including Golden
Horn Bay, and the East Bosphorus Strait (nine
samples);
• Amursky Bay, including the outer harbor of
Vladivostok (12 samples);
• Ussuriysky Bay (16 samples);
• Strelok Bay (seven samples); and
• Nakhodka Bay including Nakhodka harbor (five
samples).
As can be seen in Fig. 1, Golden Horn Bay and the East
Bosphorus Straight are relatively enclosed. Water
exchange between them and Peter the Great Bay is,
therefore, restricted. Amursky Bay is larger but is semienclosed so it is not totally free-flushing.
The most obvious pollutant inputs to Peter the Great
Bay are industrial and municipal waste waters from
Vladivostok, Nakhodka (including port facilities in
these cities and discharges from ships) and other towns
along the coastline but polluted river runoff and
dredged material dumping may also be important. The
total amount of waste waters discharged into Peter the
great Bay in 1990 was 486x 106 m 3, about 20% of which
was discharged without any treatment. As a result,
Golden Horn Bay, Amursky Bay and Nakhodka harbor
are subjected to high anthropogenic impact. Ussuriysky
Bay and Strelok Bay, on the other hand, are much less
impacted.
Ussuriysky Bay has a very wide mouth allowing free
water exchange with Peter the Great Bay. Although
there are some waste water discharges from the west
(Vladivostok) and the east coasts, as well as riverine
inputs, the pollutant load per unit area is much lower
in Ussuriysky Bay than in other areas. Strelok Bay is
used mainly by the Russian navy; therefore pressure
from population and industry in this area is relatively
small.
Keywords: Trace metals, bottom sediments, pollution,
Sea of Japan, Peter the Great Bay.
INTRODUCTION
In September 1994 the Action Plan for the protection of
the marine environment of the north-west Pacific Ocean
was signed by representatives of Japan, the People's
Republic of China, the Republic of Korea and the
Russian Federation. One of the first goals of this Action
Plan is an assessment of the environmental state of the
Sea of Japan and the Yellow Sea. Considerable progress
towards reaching this goal has been made by FERHRI
specialists over the past 15 years through comprehensive
environmental studies in the coastal zones of the Sea of
Japan. Results of some of this work have been published (Tkalin, 1992; Tkalin et al., 1993). This short
report presents recent data on variations in trace metal
concentrations in coastal sediments from Peter the
Great Bay, extending the earlier work by more intense
sampling, determination of additional elements and
radiometric dating of two cores so as to give a time
context to trace element fluxes to this area.
*To whom correspondence should be addressed.
73
74
A . V . Tkalinet al.
i
43030 '
43000 '
132 °
133 °
Fig. 1. Study areas (above) and Peter the Great Bay (below).
1--Golden Horn Bay and East Bosphorus Strait, 2--Amursky
Bay, 3--Ussuriysky Bay, 4--Strelok Bay, 5--Nakhodka Bay.
grated with a Digital VAX II/GPX graphics workstation. Concentrations were obtained by comparing
counts for each sample with those for sediment and
rock reference materials of accurately known elemental
composition. Details of this method are given in Boothe
and James (1985), including information on counting
geometry, reference materials, spikes, blanks and other
aspects of QA/QC.
The National Status and Trends Program methods
(Leuinstein & Cantillo, 1993) were used in the AAS
analysis. Briefly, 200 mg aliquots of the powdered sediment samples were weighed into Teflon 'bombs' and
completely dissolved in a mixture of nitric, hydrofluoric
and boric acids by prolonged exposure of the closed
bombs to a temperature of 130°C. Various dilutions
were made on the clear digests to bring them into the
working range of the AAS. A Perkin-Elmer Corp
model 306 flame AAS was used for Fe, Mn and Zn
analysis essentially following the manufacturer's
instructions. Other elements were determined using a
Perkin-Elmer 3030Z equipped with an HGA-600
graphite furnace and an auto sampler. Details of furnace programs, matrix modifiers, blanks, spikes, reference
materials and other QA/QC information can be found
in the reference given above. Matrix spike recovery
for all elements was almost always >90%, as were
recoveries of certified values on reference materials.
Several elements were determined by both AAS and
INAA and differences between results from the two
methods were generally < 10%.
Published data for samples from the northern part of
the Sea of Japan, as well as the D.P.R. Korea coastal
zone and elsewhere, are discussed below for comparative purposes. Sedimentation rates for our samples were
determined using 21°pb techniques by Dr G. H. Hong,
KORDI (Korean Ocean Research and Development
Institute).
MATERIALS AND METHODS
Sediment was collected by Petersen grab and the surface
layer (about 2 cm) was used for analysis. In addition,
cores were obtained using a gravity corer with plastic
liner (5 cm inner diameter) in Amursky Bay (43001.6' N,
131045.6, E) and Ussuriysky Bay (43007.4' N, 132°11.2' E).
In preparation for analysis, sediment samples were
oven dried at 105°C and ground to a fine powder.
Because no single method can reliably determine all the
elements of interest at background concentrations in
coastal marine sediment, two different analytical methods
were used in this study, instrumental neutron activation
analysis (INAA) and atomic absorption spectrophotometry (AAS).
For INAA, 0.5 g aliquots of the powdered samples
were weighed directly into plastic vials and heat sealed.
They were then irradiated for 8 h in the 1 MW TRIGA
reactor at Texas A&M University. After a 7 day cooling
period to allow Na, CI and other interfering isotopes to
decay to low levels, the samples were counted using a
hyper pure germanium detector coupled to a Nuclear
Data Corp. model 9900 multichannel analyzer inte-
RESULTS AND DISCUSSION
The main goal of the 1994 expedition was to reveal
regularities in the spatial distribution of potential
pollutant metals in bottom sediments from Peter the
Great Bay. The trace metal content of recent sediments
depends on anthropogenic inputs as well as the natural
characteristics of the sediments, especially grain size.
The major metals Fe and A1 also vary naturally with
grain size and therefore trace metals covary with these
major metals (e.g. Trefry & Presley, 1976; Presley et al.,
1992). By normalizing trace metal concentrations to
iron, the grain-size dependence can be minimized and
subtle anomalies can be detected.
Data from the present study on the trace metal content of bottom sediments are presented in Table 1. As
expected, the highest concentrations were found in
Golden Horn Bay and the East Bosphorus Strait (the
inner harbor of Vladivostok) because of the relatively
enclosed nature and the very high pollutant input to this
area. The maximum concentration of zinc was 702 ppm,
Trace metals in bottom sediments
75
Table 1. Average trace metal concentrations (ppm) and % Fe in the surface 2 cm of bottom sediments of the study area
Area
Fe
Mn
Zn
Cr
Cu
Pb
Ni
Co
Cd
Ag
Hg
Golden Horn Bay
Nakhodka Bay
Amursky Bay
Ussuriysky Bay
Strelok Bay
3.62
4.28
4.41
2.03
2.06
226
579
321
190
199
362
163
121
60
54
119
84
87
48
41
181
31
25
15
8
214
100
28
23
9a
26
44
33
15
13
10.0
13.3
12.1
5.9
5.4
3.2
0.9
0.4
0.2
0.5
1.40
0.13
0.25
0.09
0.09
1.38
0.18
0.10
0.08
0.06
aExcluding one value of 349 ppm.
and other metals were also greatly enriched over values
found outside this area, for example, lead--531, c o p p e r - 556, cadmium--7.1 and mercury--3.14 ppm. In the
inner harbor of Nakhodka maximum concentrations of
these metals were 377, 46, 61, 3.7 and 0.44 ppm respectively, also much higher than values in the more pristine
parts of the study area.
Concentrations of trace metals in some Amursky Bay
surface sediments are relatively high. At two stations
along the east coast of the bay (i.e. along the municipal
coastline where sewage outfalls are situated) zinc
reached 175 ppm, lead--55, copper---42, c a d m i u m - - l . 3
and mercury--O.36 ppm.
Ussuriysky and Strelok Bays have more sandy (i.e.
larger grain size) sediments which is reflected in a lower
iron content (Table 1) and a lower background concentration of other metals. In spite of that, very high
concentrations of zinc (184 ppm), lead (101), copper
(84) and mercury (0.46 ppm) were found in the bottom
sediments at two stations along the west coast of
Ussuriysky Bay, close to sewage outfalls and a coastal
city landfill.
Plotting distribution of measured metal concentrations versus Fe content allows one to distinguish
between natural levels of trace elements and anthropogenically enriched ones (Trefry & Presley, 1976;
Windom et al., 1989). Concentrations of some trace
metals (Ag, Cd, Hg, Pb, Cu and Zn) at the stations close
200
180
160
140
to Vladivostok and Nakhodka were much higher than
expected from metal-iron correlations (Fig. 2). On the
other hand, outside the areas of direct influence of
anthropogenic sources (about 3-5 miles) the distribution of metals can generally be explained by natural
factors. Other metals (e.g. Sc, Co, Mn or Ni) reveal
no anthropogenic influences when plotted versus Fe
(Fig. 3).
Another way to recognize anthropogenic influences is
to compare trace metal concentrations in bottom sediment of Peter the Great Bay with those in more pristine
areas of the Japan Sea. For example, in the D.P.R.K.
coastal zone (about 40 ° N) reported concentrations of
lead, copper and cadmium were 18 ppm, 8 ppm and
<0.1 ppm respectively (Tkalin, 1992), i.e. significantly
lower than those measured close to Vladivostok and
Nakhodka. The average contents of zinc (47 ppm),
nickel (13 ppm) and copper (6 ppm) in bottom sediments along the west coast of the Tatarsky Strait (about
50 ° N) in September 1992 were also lower than those
near Vladivostok and Nakhodka, especially the inner
harbor samples.
High concentrations of trace metals are often
observed in heavily populated and industrialized areas.
To illustrate this, data for different coastal areas of the
N W Pacific are presented in Table 2. According to other
reports, a very high content of lead (up to 177 ppm) was
observed in Hong Kong bottom sediments (Yim, 1984).
In Tokyo Bay the maximum concentration of lead in
1981 was 74 ppm, copper--125, c a d m i u m - - l . 9 and
mercury--0.79 ppm (Matsumoto, 1988). According to
Katoh and Suzuki (1984), highest concentrations of lead
and cadmium in bottom sediments of Tokyo and
Sagami bays were 140 and 3.0 ppm respectively. In
Dokai Bay (Japan) concentrations of cadmium and
la0
mmm
m•nm
fi ioo
18
8O
14
12
60
~10
40
,
•
2O
i
•
0
0
6
4
I
I
[
I
I
I
1
2
3
4
5
6
Fe (%)
Fig. 2. Concentrations of Zn (ppm) in bottom sediments of
Peter the Great Bay versus iron (%). Five values between 379
and 702 ppm from Golden Horn Bay were excluded.
2
t
!
0
1
i
i
p
----
i
2
3
4
5
6
Fe (%)
Fig. 3. Concentrations of Co and Sc (ppm) in bottom sediments of Peter the Great Bay versus iron (%).
76
A . V . Tkalin et al.
mercury in bottom sediments in 1990 reached 10.6 and
7.0 ppm respectively, even after the dramatic improvement in environmental controls the since 1970s (Ueda et
al., 1994).
I n s u m m a r y , c o n c e n t r a t i o n s o f trace metals m e a s u r e d
in the b o t t o m sediments n e a r V l a d i v o s t o k (in the i n n e r
harbor and Amursky Bay) are comparable with those in
highly industrialized bays in Korea and Japan (Masan
Bay, Tokyo Bay). The concentrations of zinc, lead and
mercury in Golden Horn Bay sediments are higher than
those which reportedly cause biological effects (Long &
Morgan, 1990). Concentrations of trace metals mea-
Table 2. Trace metal concentrations (ppm) and % Fe in bottom sediments of some coastal areas of the N W Pacific
Area
Fe
Mn
Zn
Cr
Cu
Pb
Ni
Co
Cd
Hg
Masan Bay (Lee & Min, 1990)
Manila Bay (Prudente et al., 1988)
Seto Inland Sea (Hirata, 1985)
Bohai Bay (Ye, 1991)
Huanghe Estuary (Zhang et aL, 1988)
3.10
3.28
3.25
3.50
0.19
561
656
879
500
438
690
136
241
74
71
100
-58
50
64
140
55
38
25
22
54
35
-22
2
53
15
49
35
47
18
11
18
---
3.0
2.2
----
0.46
--0.09
--
Table 3. Trace metal concentrations (ppm) and % Fe in the Amursky Bay sediment core
Core depth (cm)
Fe
Mn
Zn
Cr
Cu
Pb
Ni
Co
Cd
Ag
Hg
0-2
2--4
4--6
6-8
8-10
10-12
12-14
14-16
16-18
18-20
20-22
22-24
24-26
26-28
2.04
2.22
2.26
2.07
2.04
2.23
2.25
2.20
2.01
2.07
2.00
2.03
2.16
2.19
190
203
207
213
209
243
242
222
227
247
231
244
234
228
58
56
54
50
47
50
49
51
49
46
44
47
47
49
46
50
50
51
48
54
53
52
50
56
49
52
50
56
6.0
8.3
7.8
5.8
6.0
6.3
8.0
7.7
6.7
6.5
6.2
6.6
6.5
7.9
18.5
16.5
16.6
15.6
14.2
14.7
13.0
12.7
12.9
12.5
12.2
12.6
13.2
12.9
19.4
19.4
18.9
18.8
17.1
22.2
20.6
20.1
28.7
19.9
18.7
21.2
19.3
20.3
6.2
6.7
7.0
6.4
6.4
6.7
6.7
6.5
6.3
6.3
6.2
6.2
6.0
6.2
0.19
0.24
0.19
0.17
0.10
0.09
0.11
0.13
0.09
0.11
0.12
0.12
0.15
0.14
0.12
0.12
0.10
0.09
0.10
0.04
0.04
0.03
0.03
0.06
0.02
0.04
0.06
0.04
0.04
0.05
0.04
0.05
0.03
0.03
0.03
0.02
0.03
0.03
0.04
0.03
0.04
0.04
Ag/Fe Ratio
0
0
0.04
I
0.08
I
Pb/Fe Ratio
0.12
I0
I0
Depth 15
Depth 15
(cm)
(cm)
20
I
30
I
I
0.04
0.08
Cd/Fe Ratio
25
30
0.12
7
8
9
I
I
I
I
10
1
20
25
6
15
I
I
20
25
30
Za/F¢ Ratio
Fig. 4. (a) Vertical profiles of Ag and Cd (ppm) normalized by iron (%) in the Amursky Bay sediment core. (b) Vertical profiles of
Pb and Zn (ppm) normalized by iron (%) in the Amursky Bay sediment core.
77
Trace metals in bottom sediments
Table 4. Concentrations of trace metals (ppm) and % Fe in the Ussuriysky Bay sediment core
Core depth, crn
Fe
Mn
Zn
Cr
Cu
Pb
Ni
Co
Cd
Ag
Hg
0-2
2-4
4-6
6-8
8-10
10-12
12-14
14-16
16-18
18-20
20-22
22-24
24-26
26-28
28-30
2.95
2.85
2.81
2.78
2.80
2.80
2.77
2.72
2.95
3.02
3.06
3.06
2.82
2.86
2.83
254
254
259
256
303
283
299
300
306
297
305
273
308
253
218
79
66
69
67
67
63
66
63
64
64
66
64
57
56
56
67
66
68
67
65
67
66
69
66
65
65
66
68
70
70
14.0
10.1
10.3
9.2
10.6
9.2
9.5
11.1
10.1
11.0
12.7
6.4
8.8
11.0
11.1
21.2
16.9
15.6
15.5
16.4
14.0
15.1
15.2
13.6
13.7
13.9
13.1
11.8
12.2
12.7
22.1
19.9
21.1
22.1
20.9
23.6
22.6
22.5
22.3
20.9
21.3
30.5
21.7
20.8
21.7
7.0
6.9
7.3
6.8
6.7
7.2
7.2
7.0
7.1
6.9
7.1
6.3
6.4
6.6
7.0
0.39
0.41
-0.41
0.46
0.43
0.43
0.43
0.44
0.42
0.42
0.41
0.45
0.54
0.55
0.16
0.12
0.13
0.12
0.11
0.11
0.12
0.10
0.1 l
0.10
0.11
0.10
0.08
0.09
0.11
0.05
0.05
0.07
0.06
0.06
0.06
0.08
0.07
0.05
0.06
0.07
0.05
0.07
0.06
0.06
Table 5. Trace metal fluxes (mg m - 2 year -1) to bottom sediments of some coastal areas of the north Pacific
Area
Ussuriysky Bay
Amursky Bay
Tokyo Bay (Matsumoto, 1988)
Osaka Bay (Hoshika & Shiozawa, 1 9 8 6 )
Strait of Georgia (Macdonald et al., 1 9 9 1 )
Puget Sound (Bloom & Crecelius, 1987)
Sediment at
ion rate
(g cm -2 year -1)
Zn
Cu
Pb
Cd
0.12
0.17
0.12
0.11-0.28
0.17-0.89
0.354).77
71
209
-362
270-940
--
18
43
82
57
100-400
84-436
27
48
56
.
28-180
69-372
0.24
0.69
1.4
sured in Ussuriysky Bay and Strelok Bay as well as
along D.P.R.K. shelf and in Tatarsky Strait are lower
than values observed in moderately polluted areas of the
N W Pacific (e.g. Bohai Bay or Huanghe Estuary).
A sediment core was taken in the south-eastern part
of Amursky Bay and another in the central part of
Ussuriysky Bay, outside the direct influence of sewage
outfalls. Vertical profiles of Zn, Pb, Ag and Cd (normalized to iron c o n t e n t ) i n the Amursky Bay sediment
core are shown in Fig. 4, data on trace metal distribution for both cores are presented in Tables 3 and 4.
Using 21°pb dating, sedimentation rates in these cores
were estimated as 0.173 g cm -2 year- l (0.13 cm year- l)
and 0.118 g cm -2 year -1 (0.18 cm year -1) respectively
(G. H. Hong, personal communication). Therefore, the
increase in trace metal content of Amursky Bay bottom
sediments began in approximately 1945. Vertical profiles of trace metals in the Ussuriysky Bay sediment core
do not reveal a clear anthropogenic influence, probably
because human inputs of trace metals to Ussuriysky Bay
are more localized than in Amursky Bay.
Multiplying surface concentrations of trace metals
(Table 1) by sedimentation rate allows calculation of
fluxes of metals. These data are presented in Table 5
together with data of other authors. Actual average
fluxes are likely to be higher than these estimates
because sedimentation rates in the upper parts of
Amursky Bay and Ussuriysky Bay, close to river
mouths and sewage outfalls, are almost certain to be
higher than those where the cores were taken.
.
.
1.0-2.0
0.04-2.83
Ag
Hg
0.11
0.09
0.43
0.17
-0.67
.
--0.63-4.41 0.36-2.13
CONCLUSIONS
Trace metal concentrations in bottom sediments of
Peter the Great Bay showed regularities in spatial distribution and when combined with sedimentation rates
allowed an estimate of depositional fluxes to the area to
be made. Elevated levels of metals were detected in
localized areas near Vladivostok and Nakhodka, close
to municipal and industrial waste water discharges as
well as near the Vladivostok coastal landfill. The influence of these anthropogenic sources was not detected
further than a few miles. River runoff seems to be of
minor importance in the investigated areas. Compared
with highly polluted areas near Vladivostok and
Nakhodka, coastal bottom sediments in Tatarsky Strait
and the D.P.R. Korea shelf seem to be relatively clean.
Spatial distribution of trace metals outside the areas of
direct anthropogenic influence is governed by natural
factors. According to the Amursky Bay sediment core
data, increases in trace metal content of bottom sediments near Vladivostok began in approximately 1945.
ACKNOWLEDGEMENTS
The authors are very grateful to T. S. Lishavskaya,
Brad Hunter, Kuo-Tung Jiann and June Soo Park for
their assistance in sample collection, preparation and
AAS measurements, and to G. H. H o n g for 21°pb
analysis. This work became possible due to a Fulbright
78
A . V . Tkalin et al.
Program scholarship to A. V. Tkalin and the generosity
o f the Trace Element Research Lab (TERL) at Texas
A & M University.
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