anthropogenic radionuclides in kola and motovsky bays of the barents sea, russia

Journal ofEnvironmental Radioactivity 43 (1999) 77—88

Anthropogenic radionuclides in Kola andMotovsky Bays of the Barents Sea, Russia

Genady G. Matishov!, Dmitry G. Matishov!,Alexey A. Namjatov!, JoLynn Carroll",*, Salve Dahle"

! Murmansk Marine Biological Institute, 17 Vladimirskaya St. Murmansk, 183010, Russia" Akvaplan-niva, Fiolvn. 15, N-9005 Troms~, Norway

Received 10 June 1998; received in revised form 25 August 1998; accepted 3 September 1998

Abstract

Russia’s military and civilian nuclear powered maritime fleets operate in the Kola andMotovsky Bays on the northwest Arctic coast of Russia. Levels of anthropogenic radionuclideswere measured in sediment grab samples collected from approximately 100 stations in areasnear military and civilian nuclear installations and in the open waters of the two bays. Inmost areas, radionuclide levels are similar to those reported for other Arctic seas:137Cs"1—24 Bq kg~1 d.w., 60Co"(1 Bq kg~1 d.w. and 239,240Pu"0.8—1.6 Bq kg~1 d.w.However, the presence of 60Co (up to 27 Bq kg~1 d.w.) indicates that minor leakage ofradioactive waste has occurred near several military installations. Sites where leakage isdetected include Pala, Sayda, Olenya and Ekaterininskaya Bays in the Kola Bay and Zapad-naya Litsa in Motovsky Bay. 137Cs levels of 40—50 Bq kg~1 d.w. and 239,240Pu levels of up to2.2 Bq kg~1 d.w. were measured near several military installations but these levels do notindicate leakage as the source.

Some of the highest 60Co activities were detected in sediments collected near the civiliannuclear installation, Atomflot. The sediments also contained higher 137Cs activities comparedto samples from other regions of the study area with similar particle size distributions. Routinedischarges of purified radioactive waste from the Atomflot facility are the likely source of 60Coand enhanced 137Cs levels. With this investigation, we have detected evidence of radioactivewaste leakage in the marine environment, but the environmental impact on the bays has beenminimal. ( 1999 Elsevier Science Ltd. All rights reserved.

Keywords: Nuclear waste; Radioactivity; Kola Peninsula; Marine sediments; 137Cs; 239,240Pu;60Co

*Corresponding author. Tel.: (47) 77 68 52 80; fax: 47 77 68 05 09; e-mail: [email protected].

0265-931X/99/$ — see front matter ( 1999 Elsevier Science Ltd. All rights reserved.PII: S0265-931X(98)00096-4

1. Introduction and background

The Kola Peninsula in northwest Russia is a 100 000 km2 area of tundra, forest andlow mountains between the White Sea and the Barents Sea. Its proximity to theAtlantic Ocean and year-round ice-free harbours made it a suitable location forRussian military bases after the Second World War. During the Cold War, develop-ment and construction of nuclear submarines and various missile systems receivedhigh priority. Today there are a number of naval bases and shipyards situated in theinlets and small bays of Motovsky and Kola Bays (Fig. 1). This region now has thehighest concentration of nuclear reactors, active and derelict, in the world (Yablokovet al., 1993). In addition to military installations, a civilian nuclear icebreaker base,Atomflot, is located in Kola Bay.

Early in the development of the region as a major port, radioactive waste wasdischarged to the sea. Following the ratification of the 1972 Convention on thePrevention of Marine Pollution by Dumping of Wastes and Other Matter whichprevented further releases to the sea (Sjoeblom & Linsley, 1995), all liquid and solidnuclear wastes generated at the port were stored on land.

Waste inventory estimates for the region are difficult to obtain and verify due to thesecrecy surrounding military operations in the Kola region. Bradley et al. (1997)report solid and liquid waste inventories at Northern Fleet military installations of1100 Ci (40.7]1012 Bq). In addition, the civilian icebreaker base RTP Atomflotintentionally discharges 500 m3 annually (up to 1.5]109 Bq yr~1) of purified radioac-tive waste into Kola Bay (Atomflot Laboratory, pers. comm.). The vast majorityof radioactive material found in this region is associated with naval and civiliannuclear reactors. In a report prepared for the Arctic Monitoring and AssessmentProgram on Arctic Radioactivity, Strand et al. (1997) estimate a total 137Cs#90Srradionuclide activity of 2.2]1018 Bq for the 131 military#civilian nuclear reactorsin the region.

In the adjacent Arctic Seas, the primary sources of radioactivity are discharges fromEuropean reprocessing plants, global fallout from weapons testing in the 1950s and1960s, run-off from major Siberian river catchment areas, Chernobyl fallout, andfallout from underwater nuclear tests conducted at Novaya Zemlya (Aarkrog, 1994).Among these sources, discharges from the European reprocessing plants are theprimary source of 137Cs (Kershaw & Baxter, 1995). The most important source of239,240Pu is global fallout. 60Co is not widely present except in close proximity torelease areas, such as the underwater nuclear test site at Novaya Zemlya (Smith et al.,1995). Investigations conducted in the open sea areas adjacent to the Kola region (e.g.Barents, Kara, Pechora and White) have not shown radionuclide levels that could notbe explained by these well-known sources (Smith et al., 1995, Strand et al., 1994;Hamilton et al., 1994). Contaminated marine sediments have been found in severalshallow bays along the coast of Novaya Zemlya where objects containing radioactivewaste were dumped by the Former Soviet Union (Nikitin et al., 1995; Salbu et al.,1995; Osvath et al., 1995).

There has been great concern that nuclear-related activities along the Kola coasthave resulted in unintentional discharges of radionuclides into the surrounding land,

78 G.G. Matishov et al./J. Environ. Radioactivity 43 (1999) 77—88

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G.G. Matishov et al./J. Environ. Radioactivity 43 (1999) 77—88 79

air and sea. Until now, information on the levels of waste-related radionuclides in thesea environment within close proximity to the military and civilian installations ofKola and Motovsky Bays has not been available. In 1996, a preliminary assessment ofthe current environmental situation was conducted (Matishov, 1997). The purposeof the assessment was to identify the presence of anthropogenic radionuclides in themarine environment and to measure concentrations in various environmental com-partments. In this paper we present data on sediment samples collected and analysedfor the radionuclides 137Cs, 239,240Pu and 60Co. Principal areas of investigation werethe small inlets, Big Motka, Kutovaya, Titovka, Western Litsa, Ara and Ura inMotovsky Bay and Saida, Olenya, Pala, and Ekaterininskaya in Kola Bay (Fig. 1).

2. Materials and methods

In May—June 1996, the Murmansk Marine Biological Institute (MMBI) carried outan expedition to Kola and Motovsky Bays. Sediment samples were retrieved from theseabed using a Van Veen grab sampler that penetrated the seabed to a depth ofapproximately 10—15 cm. Sediment samples were collected in water depths of30—180 m at locations 1—4 km from the nearest nuclear bases. Samples retrieved fromthe grab sampler (0.5—1 kg) were stored in plastic bags and refrigerated until transferto the laboratory. 137Cs and 60Co activities were determined at approximately 100stations. 239,240Pu activities were determined at 14 stations.

3. Radioanalytical approach

3.1. 137Cs and 60 Co determinations

Radiochemical analyses were performed at the Khlopin Radium Institute(St. Petersburg). 137Cs and 60Co were measured on a low level, lithium-driftedgermanium (Ge(Li)) gamma spectrometry system. Prior to analysis, each sample wasdried, then ground and mixed thoroughly. Samples (0.1—0.3 kg d.w.) were placed inspecial cylindrical containers for gamma measurements. Routine instrument calib-ration is performed at the Khlopin Radium Institute twice per month using standardspurchased from the U.S. Department of Energy. Detector performance is also evalu-ated during intercomparison exercises conducted by the International Atomic EnergyAgency. Instrument detection limits for both 137Cs and 60Co are 1 Bq kg~1 d.w(herein Bq kg~1"Bq kg~1 d.w.). Errors for 137Cs and 60Co activities are (10% forsamples '10 Bq kg~1; (40% for samples 5—10 Bq kg~1 and (50% for samples1—5 Bq kg~1.

3.2. 239,240Pu determinations

The samples were mixed with oxalic acid and ashed at 500°C for 24—48 h to destroyorganic material. 239,240Pu purification was performed using standard ion exchange


chromatography techniques. Sample residues were leached with 8M HNO3

afteraddition of 242Pu as a yield tracer. Transuranic elements were separated from samplesby coprecipitation on iron hydroxide. Plutonium was isolated by adsorption on ananion-exchange column preconditioned with 8M HNO

3and subsequently eluted

with HCl. For a good purification of the Pu eluate, a second anion exchange columnwas processed. The final elution of Pu was done in 10 M HCl and 0.1 M NH

4I

solution. The eluate was evaporated and further purified before electrodepositiononto stainless steel discs (Hallstadius, 1984). Certified alpha spectrometry systemswere used to determine 239,240Pu activities to within (10% measurement errors.The reliability of the procedure was confirmed during intercomparison exercises usingthe certified reference material, IAEA Soil-6.

4. Results

The distributions of radionuclides in bottom sediment samples are graphicallydisplayed in Figs. 2—4, respectively. Samples from stations throughout the region were

Fig. 2. Surface sediment concentrations of 137Cs. Errors are (10% for samples '10 Bq kg~1; (40%for samples 5—10 Bq kg~1 and (50% for samples 1—5 Bq kg~1.


Fig. 3. Surface sediment concentrations of 239,240Pu. Measurement errors are less than 10%.

analysed for the radionuclides, 137Cs, 239,240Pu and 60Co but 60Co was detected onlynear the military and civilian bases. Average and maximum activities of 137Cs and60Co for major inlets and within open waters of Kola and Motovsky Bays are given inTable 1. 239,240Pu and 239,240Pu/137Cs activity ratios are presented in Table 2.

Radionuclide levels in Motovsky Bay exhibit the following distributions. 137Cslevels of 0.7—30 Bq kg~1 were observed in the outer part of Western Litsa Inlet inbottom sediments ranging from fine-grained to sandy material. Bottom sediments inthe outer parts of Ara and Ura Inlets had 60Co levels of 0.5—1.0 Bq kg~1 and 137Cslevels of 0.6—14 Bq kg~1. Radionuclide activities in bottom sediments from an adjac-ent inlet (Titovka Inlet) were similar in areas both offshore (137Cs"1—10 Bqkg~1;60Co"0.5—1.0 Bq kg~1) and nearshore (137Cs"5—14 Bq kg~1; 60Co"0.7—1.0Bq kg~1). These inlets exhibit no unusual radionuclide levels when compared withradionuclide levels from open water stations. Zapadnaya Litsa Inlet, in AndreevaBay, is the location of one of the largest nuclear submarine bases found in this region.The highest 137Cs activity observed in this study (48 Bq kg~1) was detected in thisinlet. Maximum 60Co levels in Zapadnaya Litsa Inlet were 4.0 Bq kg~1.


Fig. 4. Surface sediment concentrations of 60Co. Errors are (10% for samples '10 Bq kg~1; (40%for samples 5—10 Bq kg~1 and (50% for samples 1—5 Bq kg~1.

In Kola Bay, levels of artificial radionuclides generally increase with decreasingdistance to the nuclear bases. 60Co (0.7—12 Bq kg~1) was detected in bottom sedi-ments from Saida Inlet, 2—3 km from sites used for storage of reactor compartmentsfrom nuclear submarines. 137Cs levels in Saida Bay ranged from 3 to 34 Bq kg~1.The 239,240Pu activity, determined for one station location from Saida Bay was1.6 Bq kg~1. Radionuclide levels in sediments from Olenya Inlet, 800 m from the‘Nerpa’ ship repair works were: 137Cs"2—14 Bq kg~1, 60Co"1—12 Bq kg~1 and239,240Pu"1.6 Bq kg~1. High levels of 60Co (22—24 Bq kg~1) were found in Pala andEkaterininskaya Inlets near Polyarny in combination with slightly higher 137Cs(15—22 Bq kg~1), and 239,240Pu (2.2 Bq kg~1) levels. Sediments collected adjacentto the civilian nuclear icebreaker base, Atomflot, exhibited the highest 137Cs(43.0 Bq kg~1) and 60Co (27.0 Bq kg~1) activities detected in samples from Kola Bay.The obvious source of elevated radionuclide levels in the vicinity of Atomflot isroutine discharges of purified nuclear waste.


Table 1Concentrations of 137Cs and 60Co in surface bottom sediments in areas of the Kola and Motovsky Bays(Bq kg~1 d.w.)

Area Number of 137Cs 60Cosamples

Aver. S.d. Max Aver. S.d. Max

Near-field Barents Sea 2 6.2 7.2 (1

Kola BayOpen water 24 12.6 5.0 24.5 (1Area of ‘ATOMFLOT’ 82 18.0 6.2 43.0 0.8 1.4 27.0Pala Bay 1 20.3 22.9Olenja Bay 4 7.0 4.3 14,0 4.5 11.5Ekaterininskaya Bay 2 13.3 14.6 13.2 24.0

(Polyarny)Saida Bay 8 9.8 10.5 34.1 2.7 4.0 12.0Vaenga Bay (Severomorsk) 10 11.1 5.5 18.9 (1

Motovsky BayOpen water 13 3.8 2.9 10.1 (1Zapadnaja Litsa 9 16.7 15.6 48.4 0.6 1.4 4.0Ara Bay 5 4.2 4.8 11.0 (1Ura Bay 8 4.3 4.4 13.8 (1

Table 2Concentrations of 239,240Pu and 239,240Pu/137Cs activity ratio in surface bottom sediments in the Kola andMotovsky Bays

Area Number of NuclideSamples

239,240Pu(Bq/kg d.w.) 239,240Pu/137Cs

Middle part of the Kola Bay 1 1.65$0.18 0.104Northern part of the Kola Bay 1 1.51$0.30 0.132Area of ‘ATOMFLOT’ 8 0.8 $0.15 0.019—0.100Pala Bay 1 2.20$0.40 0.108Saida Bay 1 1.58$0.29 0.122Zapadnaja Litsa 1 2.01$0.31 0.042Ura Bay 1 1.30$0.30 0.094

5. Discussion

It has been previously impossible to obtain data on the levels and distributions ofanthropogenic radionuclides near military installations operated by the RussianNorthern Fleet. In this preliminary investigation of the environmental situation in theKola region, we have presented radionuclide data from approximately 100 sites inMotovsky and Kola Bays, including sites in close proximity to several militaryinstallations. The levels of 137Cs, 60Co and 239,240Pu are relatively low throughout


the region, but leakage of radionuclides into the marine environment is detected insome areas. The presence of 60Co in sediment samples collected near several militaryinstallations supports this conclusion. Although 60Co (t

1@2"5.27 year) was pre-

viously introduced to Kola and Motovsky Bays by global fallout, 60Co derived fromthis source will have decayed to insignificant levels. 60Co also exhibits a strong affinityfor particles and detection of this radionuclide is only possible within close proximityto a point of release. Thus, high 60Co activities unequivocally indicate that someleakage of radioactive waste has already occurred in the bays.

High 60Co activities are present mainly in Kola Bay (Table 1). In Motovsky Bay,60Co activities are generally below detection ((1 Bq kg~1) except in ZapadnayaLitsa where high activities of both 137Cs and 60Co are observed at a few locations. Wehave identified the following areas where anomalous radionuclide activities are found:Atomflot area, Pala, Sayda and Olenya Bays, and Ekaterininskaya Bay in Kola Bayand Zapadnaya Litsa in Motovsky Bay. Leakages of artificial radioactivity fromnuclear storage sites and other nuclear activities in these areas are believed to be thecause of these uncharacteristic radionuclide activities.

Unlike 60Co, 137Cs increases caused by leaking radioactive waste are not immedi-ately apparent in these data. We did observe a general trend of increasing 137Csactivities with decreasing distance toward the military installations and our 137Cslevels are similar to levels reported for nuclear waste dumping sites in Tsivolky Bayand other dumping sites in the bays of Novaya Zemlya (Nikitin et al., 1995; Salbu etal., 1995; Osvath et al., 1995). However, the highest levels of 137Cs detected insediments from Kola and Motovsky Bays are only 40—50 Bq kg~1. These 137Csactivities are not much higher than 137Cs activities of up to 30 Bq kg~1 which havebeen reported as typical for sediments from Arctic Seas (e.g. Baskaran et al., 1996;Hamilton et al., 1994; Strand et al., 1994).

Rather than contamination from leaking radioactive waste, other well-knownsources and geochemical processes may explain the 137Cs activities observed insediments from the different parts of the bays. For example, scavenging of runoff-borne global and Chernobyl fallout may result in near-shore enhancements of 137Cs.Particle characteristics (size, mineralogy, cation exchange capacity) favoring increasedsorption of 137Cs may also explain these data (Duursma & Carroll, 1995). Indeed,particle size does explain some of the observed variation in 137Cs activities. 137Csactivities are higher in samples containing higher percentages of clay#silt particles asdemonstrated in Fig. 5. Overall, the evidence is not strong enough to conclude thatleakage from military installations is responsible for enhanced 137Cs activities insediments from the bays.

The one exception may be near the civilian nuclear icebreaker base, Atomflot. Someof the highest activities of both 137Cs and 60Co were found in sediment samples fromthe Atomflot area (Table 1). Also, if we compare sediments having similar percentagesof clay#silt particles from the Atomflot area with samples from other areas (Fig. 5),137Cs activities in sediments from the Atomflot area (Kola Bay South) are noticeablyhigher. Although these 137Cs activities also may be the result of natural variations insediment composition, the trend is striking. It is plausible that routine discharges ofpurified radioactive waste from the Atomflot facility are responsible. With a ten-fold


Fig. 5. Variations in 137Cs with sediment grain size (clay#silt fraction) for different areas of the Bays. Thecircle delineates data from Kola Bay south. The Atomflot facility routinely discharges purified radioactivewaste into this area of the bay.

increase in discharges from Atomflot planned for 1999 (Atomflot Laboratory, pers.comm.), this trend should become even more apparent within the next few years.

239,240Pu activities, determined for some sites in the inlets of Kola and MotovskyBays are not significantly different from the levels expected from global sources of239,240Pu (Baskaran et al., 1996). 239,240Pu activities are mainly the result of atmo-spheric fallout from nuclear weapons testing performed in the 1950’s and 1960’s(Holm et al., 1986). In general, 239,240Pu/137Cs activity ratios similar to ratiosobserved in the Kara Sea (Baskaran et al., 1996) were observed in the open waters ofKola and Motovsky Bays. The ratio of 239,240Pu activity to 137Cs activity is oftena useful indicator of possible sources of radioactivity to marine sediments (Smith et al.,1995), however, we are unable to clearly distinguish among different source contribu-tions from the few data we have for Kola and Motovsky Bays. Thus there is nocompelling evidence to suggest that any new anthropogenic sources have contributedadditional 239,240Pu to sediments in the bays.

Currently, the impact on the bays from radioactive waste discharges appears to beminimal. We therefore, do not expect any significant increases in radionuclide activityin the adjacent Arctic Seas as a result of exchanges of water or sediment from Kolaand Motovsky Bays. Indeed, 137Cs activities determined in sediment samples col-lected in the Barents Sea, just outside of the bays, are only 6.2—7.2 Bq kg~1 and 60Cowas not detected (Table 1).


The radiological implications of these data are presented in a follow-up paper(Matishov et al., submitted) which shows that there does not appear to be anyincreased radiological risk to humans as a result of the current situation in the baysand inlets of Kola and Motovsky Bays.

The outcome of this investigation, showing little impact on Kola and MotovskyBays, is obviously welcome. The 137Cs, 239,240Pu and 60Co activities detected in thesemarine sediments represent only a very minor fraction of the total amount ofradioactivity currently stored in the Kola region (Yablokov et al., 1993). Anddespite these findings, there will continue to be concerns regarding proper handlingof nuclear waste materials, the integrity of storage containers, and current storagelocations in the Kola region. Therefore continued investigation is essential inorder to detect any future changes in the conditions of these bays. Although wehave established a general picture of the radioactivity situation in Kola andMotovsky Bays, our findings are based only on analyses of seabed grab samples.Determinations of radionuclide inventories in sediment deposits are needed to obtaina better idea of the magnitude and extent of both past and present leakage from thevarious installations. The determination of sedimentation rates would help to estab-lish a more detailed chronology of past leakage events and to determine if the leakageproblems are accelerating with time. The planning of these investigations is currentlyunderway.

6. Conclusions

(1) Sediment radionuclide levels (137Cs, 60Co,239,240Pu) are low in most areas of Kolaand Motovsky Bays.

(2) Co activities in sediments indicate that minor leakage of radioactive waste hasoccurred in some areas adjacent to military and civilian nuclear installations.

(3) From these data it is clear that the impact on the marine environment fromleakage of radioactive waste, thus far, has been minimal.

(4) As the information reported here is based on analyses of sediment grab samples,follow-up investigations needed for this region include the determination ofradionuclide inventories and an examination of the chronology of past leakageevents.

Acknowledgements

Financial support for this investigation was provided by the Murmansk MarineBiological Institute of the Russian Academy of Sciences and by Akvaplan-niva. Wethank Dr. John Smith, Bedford Institute of Oceanography and three anonymousreviewers for useful suggestions on this manuscript. We also wish to acknowledge theexcellent analytical work performed by the Khlopin Radium Institute (St. Petersburg,Russia) under the direction of Prof. Yu. V. Kuznetsov.


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anthropogenic radionuclides in kola and motovsky bays of the barents sea, russia

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