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IAEA-TECDOC-1094

XA9951887-2^0?

Marine pollution

Proceedings of a symposium held in Monaco, 5-9 October 1998 organized by the International Atomic Energy Agency (IAEA) co-sponsored by the Intergovernmental Oceanographic Commission (IOC) of UNESCO, the United Nations Environment Programme (UNEP) and the International Maritime Organization (IMO) in co-operation with the Commission Internationale pour {'Exploration Scientifique de la Mer Mediterranee (CIESM)

INTERNATIONAL ATOMIC ENERGY AGENCY /A

July 1999

3 0 - 4 1

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The originating Section of this publication in the IAEA was:

Radiometrics Section International Atomic Energy Agency

Marine Environment Laboratory B.P. 800

MC 98012 Monaco Cedex

The IAEA does not normally maintain stocks of reports in this series.

However, copies of these reports on microfiche or in electronic form can be obtained from INIS Clearinghouse

International Atomic Energy Agency Wagramer Strasse 5

P.O. Box 100

A-1400 Vienna, Austria E-mail: CHOUSE® IAEA.ORG

URL: http://www.iaea.org/programmes/inis/inis.htm

Orders should be accompanied by prepayment of Austrian Schillings 100,- in the form of a cheque or in the form of IAEA microfiche service coupons which may be ordered separately from the INIS Clearinghouse.

MARINE POLLUTION IAEA, VIENNA, 1999 IAEA-TECDOC-1094

ISSN 1011-4289

©IAEA, 1999

Printed by the IAEA in Austria

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FOREWORD

The marine environment - understanding and protecting for the future were at the forefront of the International Symposium on Marine Pollution convened in Monaco from 5 to 9 October 1998, as one of the major events of the UN International Year of the Oceans. The symposium was hosted by the Principality of Monaco on the occasion of the 150th anniversary of the birth of Prince Albert 1st of Monaco, "the Navigator Prince", one of the world's leading pioneers in oceanographic studies. The symposium was organized by the International Atomic Energy Agency, co-sponsored by the Intergovernmental Oceanographic Commission (IOC) of UNESCO, the United Nations Environment Programme (UNEP), the International Maritime Organization (IMO) and the Commission Internationale pour 1'Exploration Scientifique de la Mer Mediterranee (CIESM). The new premises of the Marine Environment Laboratory in Monaco were officially inaugurated during the week of the symposium. Over 400 international experts from 61 Member States and 8 international organizations delivered 114 oral presentations in plenary and parallel sessions and made 215 poster presentations.

New achievements were reported in identifying the sources of pollution, on the behaviour and fate of contaminants in seawater, biota and sediments, on the use of radioactive and non-radioactive tracers for studies of transport and circulation processes in the world's oceans and seas, on studies of radioactive waste dumping sites and nuclear weapons test sites, on local, regional and global computer modelling of the transport of contaminants and on many other topics in marine pollution.

New developments in high sensitivity analytical measurements of contaminants with emphasis on nuclear and isotopic methods were also presented. Information on global and regional marine pollution studies programmes was given and participants had the chance to interact with leading experts in the field and to discuss future trends in marine pollution studies.

A ministerial meeting of the Black Sea countries organized in the framework of the IAEA TC Regional Project RER/2/003 — Marine Environmental Assessment of the Black Sea Region — was also held during the first three days of the symposium. Environmental ministers signed the Black Sea Declaration, an important document for future collaboration in the region. The Declaration stresses the important role the IAEA plays in assisting Member States in the Black Sea region by upgrading their capabilities for the assessment of the marine environment.

This TECDOC contains some of the papers submitted on issues falling within the thematic scope of the symposium which were presented in oral and poster presentations. The papers are in one of the two working languages, English or French. Several papers presented orally at the symposium have been submitted by the authors for publication in a Special Issue of the journal "The Science of the Total Environment", published by Elsevier.

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EDITORIAL NOTE

In preparing this publication for press, staff of the IAEA have made up the pages from the original manuscripts as submitted by the authors. The views expressed do not necessarily reflect those of the IAEA, the governments of the nominating Member States or the nominating organizations.

Throughout the text names of Member States are retained as they were when the text -was compiled.

The use of particular designations of countries or territories does not imply any judgement by the publisher, the IAEA, as to the legal status of such countries or territories, of their authorities and

institutions or of the delimitation of their boundaries.

The mention of names of specific companies or products (whether or not indicated as registered) does not imply any intention to infringe proprietary rights, nor should it be construed as an endorsement or recommendation on the part of the IAEA.

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CONTENTS

Temporal variations in plutonium and americium inventories in the northwestern

Mediterranean Sea and their relation to vertical particulate flux (IAEA-SM-354/7)... 1 S.W. Fowler, V.E. Noshkin, J. La Rosa, J. Gastaud

Radioactive tracers in the Black Sea: An overview (IAEA-SM-354/8)... 8 K.O. Buesseler

Teneurs en metaux traces des sediments de surface du Lac Sud de Tunis avant

restauration(IAEA-SM-354/14) ... 13 J. Ben Souissi, J. Zaouali, S. Aouij, E. Orlando, M. Mazghouni, M. Rezig

Long-term loss rates of radioisotopes of cobalt, zinc, ruthenium, caesium and silver by

Mytilus edulis under field conditions (IAEA-SM-354/17)... 19 H. Dahlgaard, C. Nolan

Temporal and spatial responses of the bioindicator Fucus to discharges of 99Tc in the

eastern Irish Sea (IAEA-SM-354/18)... 25 P. McDonald, RG. Busby, M. McCartney

Shells ofNerita gastropod bio-monitors of heavy metal pollution around the

Indian Ocean (IAEA-SM-354/20)... 31 ML Badran

Effects of nuclear and non-nuclear pollutants on marine ecosystems (IAEA-SM-3 54/22)... _... 38 G.G. Polikarpov

Riverine transport of Cs-137 and Sr-90 into the Black Sea after Chernobyl accident

(data analysis and methodological aspects of monitoring) (IAEA-SM-354/23)... 44 V. V. Kanivets, O. V. Voitsekhovitch, B.F. Khrystyk

Application of the spectrometric and radiochemical techniques in analyzing

environmental samples from the Bulgarian Black Sea region (IAEA-SM-354/25)... 52 B.S. Veleva, G. Mungov, N. Galabov, K. Kolarova, T. Guenchev

Present level of contaminants in the Romanian Black Sea sector (IAEA-SM-3 54/26)... 58 A.S. Bologa, M. Apas, A. Cociasu, E. Cuingioglu, V. Patrascu, I. Pecheanu,

V. Piescu, L. Popa

Oxygen-18, deuterium and tritium in the Black Sea and the Sea of Marmara

(IAEA-SM-354/27)...64 E. Ozsoy, I. Salihoglu, D. Rank

Chronic oil pollution in the Bosphorus, Sea of Marmara and Dardanelles

(IAEA-SM-354/28)...73 K.C. Guven, S. Unlii, E. Okus, E. Dogan

The dynamics of nutrient enrichment and primary production related to the recent

changes in the ecosystem of the Black Sea (IAEA-SM-3 54/29)... 78 A. Yilmaz, M. Yayla, I. Salihoglu, E. Morkoc

LAEA-MEL's AQCS programme for marine radioactivity measurements (IAEA-SM-354/31)... 87 P.P. Povinec, J. Gastaud, M.K. Pham

Analytical quality control for Spanish environmental laboratories using the

ISO/IUPAC/AOAC protocol (IAEA-SM-354/32)...94 L. Romero, L. Ramos, R Salas, R Bojanowsky, R Dekner, Z. Radecki

Fresh biological reference materials - use in inter-laboratory studies and as CRMs

(IAEA-SM-354/33) ..„...„...„..„„.„...„...„„„„....„...„.„„...„„..„...„... 100 J. De Boer

Historical levels of "Tc in the Irish Sea (IAEA-SM-354/44)... 105 M. McCartney, K. Rajendran

Cadmium, lead and organic matter distribution in coastal sediment from the

Adriatic Sea (IAEA-SM-354/49) „...„....„..„„„...„...„„...„„...„...„..„.„„„„.„„.„ Ill I. Ujevic, D. Bogner, A. Baric

Accumulation of heavy metals in sediments of marine environments along the

southwest coast of India (IAEA-SM-354/51)... 117 B.R Manjunatha, P.A. Yeats, J.N. Smith, R Shankar, A.C. Narayana, T.N. Prakash

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Determination of 240Pu/239Pu isotope ratios in Kara Sea andNovaya Zemlya sediments

using accelerator mass spectrometry (IAEA-SM-3 54/59)... . . . 123 D.H. Oughton, L. Skippenid, B. Salbu, L.K. Fifield, R.C. Cresswefl, J.P. Day

Organochlorine pollutants level in teleost fish and bivalve from Egyptian

Mediterranean coast and Nile estuary (IAEA-SM-354/61)... 129 A.M.A. Abd-Allah

Persistent organochlorine pollutants (POPs) in coastal environments of

southeast Gulf of Mexico (IAEA-SM-354/63)... 135 A. Vazquez-Botello, G. Diaz-Gonzalez, L. Rueda-Quintana

Fate of 14C-labelled compounds in marine environment (IAEA-SM-354/64)... 139 S.P. Kale, K Raghn, P.D. Sherkhane, N.B.K. Murthy

An integrated strategy for biological effects monitoring in Scottish coastal waters

(IAEA-SM-354/70)... 145 R,A. Park, J. Dobson, L. Richardson, A. Hill

Metallothionein as biomarker of mussel exposure to heavy metals (IAEA-SM-3 54/71)... 151 B. Raspor, M. Erk, J. Pavicic, D. Juric, Z. Kwokal, N. Odzak

Ecotoxicity studies in Jamaican environment I. Toxiciry, bioaccumulation,

elimination and tissue partitioning of ethoprophos by the fish Tilapia in brackish

water microcosm (IAEA-SM-354/73)... 157 D.E. Robinson, A. Mansingh

Lagoon sediment radioactivity in Polynesian French nuclear test sites

(IAEA-SM-354/78)... 161 J.C. Millies-Lacroix, R. Chiappini, G. Le Petit

The production and dissolution of nuclear explosive melt glasses at underground

test sites in the Pacific region (IAEA-SM-354/81)... 169 D.K Smith, W.L Bourcier

Determination of polycyclic aromatic hydrocarbons in mussels and sediments from

the northern Adriatic Sea (IAEA-SM-354/84)... 175 M. Notar, H. Leskovsek, J. Faganeli

Responding to the Sea Empress oil spill (IAEA-SM-354/86)... 177 D.RP. Leonard, RJ. Law, C.A. Kelly

Assessment of phenols and oil pollution in the eastern Levantine (winter 1992)

(IAEA-SM-354/87)... 183 S. Noureddin, A.K. Youssef, F. Abousamra, H. Youssef

Modelling the transport of sediments and plutonium from the Mururoa lagoon

(IAEA-SM-354/89)... 187 R. Rajar, D. Zagar

Long range transport of 129I and 137Cs in the Nordic Seas and the Arctic Ocean

(IAEA-SM-354/91)... 193 M.J. Karcher, I.E. Harms, J.N. Smith

Three dimensional simulation of radionuclides dispersion in the stratified estuaries

(IAEA-SM-354/93)... 199 L. Koziy, N. Margvelashvili, V. Maderich, M. Zheleznyak

MEAD—The development of a long-term dispersion model for shelf seas

(LAEA-SM-354/94)...205 S. Clarke, J.A. Goshawk

A Monte Carlo approach in quality assurance of gamma spectrometric measurements

of marine samples (IAEA-SM-354/96)...211 C. Dovlete, P.P. Povinec

Marineoligotrophy and element biogeochemistry (IAEA-SM-3 54/97)... ... 221 RA. Jeffree, R. Szymczak

The use of natural 14C as a tracer to identify the incorporation of younger material into the organic component of sediments from the Carpentaria Basin, Australia

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Worldwide redistribution of 129Iodine from nuclear fuel reprocessing facilities:

Results from meteoric, river, and seawater tracer studies (IAEA-SM-3 54/101)... 231 J.E. Moron, S. Oktay, P.H. Santschi, D.R. Schink, U. Fehn, G. Snyder

Carbon isotopes in SOM, POM and DOM from Dutch coastal waters and estuaries

(IAEA-SM-354/103)...237 L. Megens, J. van der Plicht, J. W. de Leenw

The AMS analysis of 129I and 135Cs: Development of tools for oceanographic

tracing and pollution source identification (IAEA-SM-354/105)... 243 X-L. Zhao, W.E. Kieser, A.E. Litherland, J.N. Smith, S.W. Fowler, J-C. Miquel

Measurements of radiocarbon in the NW Pacific Ocean and its marginal seas

(IAEA-SM-3 54/107)...249 A.J.T. Jull, G.S. Burr, C. Courtney, P.P. Povinec, O. Togawa

Plutonium isotope ratios in environmental samples from Thule (Greenland) and the

Techa River (Russia) measured by ICPMS and a-spectrometry (IAEA-SM-354/109)... 254 H. Dahlgaard, Q.J. Chen, S. Stiirup, M. Eriksson, S.P. Nielsen, A. Aarkrog

Radioecological assessment of the consequences of contamination of Arctic waters —

Update on the progress of the EC-supported Armara project (IAEA-SM-3 54/112)... 260 P.I. Mitchell

Marine radioactivity studies in the world oceans (MARS) (IAEA-SM-354/114)... 262 P.P. Povinec, O. Togawa

The global ocean observing system (GOOS): New developments (IAEA-SM-354/116)... 268 C.P. Summerhayes

"Mussel Watch" and chemical contamination of the coasts by polycyclic

aromatic hydrocarbons (IAEA-SM-354/117)...273 J. W. Farrington

Global assessments of the state of the marine environment: Contemporary initiatives

(IAEA-SM-354/119)...279 J.M. Bewers, R.G. F. Boelens

Modelling the distribution of 90Sr and 137Cs in the Mediterranean Sea

(MTPH-MATER)(IAEA-SM-354/120)...285 J.A. Sanchez-Cabeza, M. Ortega, F. Fernandez, J. Tintore, A. Monaco

90Sr, 137Cs, 238Pu, 239+240pu and 24IAm in matrices of the Terra Nova Bay ecosystem (Antarctica) (IAEA-SM-354/lP)...291 F. Nonnis Marzano, C. Triulzi, G. Jia, D. Capra

High scavenging rates in the western Arctic Ocean revealed by TIMS measurements of natural radionuclides (IAEA-SM-3 54/2P)...294 H.N. Edmonds, S.B. Moron, H. Cheng, J.A. Hoff, R.L. Edwards, J.N. Smith

Radioecological studies in the Barents Sea (IAEA-SM-354/4P)... 296 H.-J. Kettermann, G. Kanisch, A. Kruger, M. Vobach

239'240Pu, 137Cs and 90Sr in bottom sediments of the Kara Sea. The attempt to reconstruct rate of the radionuclides supply to bottom sediment in the past (IAEA-SM-354/6P)... 298 Y.U.V. Kuznetsov, V.K. Legin, A.V. Stepanov, V.N. Strukov, A.E. Shishlov, Yu.V. Savitsky

Real and alleged hazard of radioactive contamination of seas caused by activities of Russian

nuclear fleets (IAEA-SM-354/7P)... 301 S.A. Lavkovsky

Physico-chemical speciation of plutonium in Arctic shelf waters at Thule, NW Greenland

(IAEA-SM-354/8P)... 303 C.A. McMahon, L. Leon Vintro, P.I. Mitchell, H. Dahlgaard

The use of 59Ni, 99Tc and 236U to monitor the release of radionuclides from objects containing spent nuclear fuel dumped in the Kara Sea (IAEA-SM-354/9P)... 305 M.E. Mount, D. W. Layton, T.F. Hamilton, M. Lynn

Radioactive contamination of the seas washing the territory of Russia (1961-1966)

(IAEA-SM-3 54/1 OP)...307 S.M. Vakulovsky, A.I. Nikitin, V.B. Chumichev

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The IAEA inventory databases related to radioactive material entering the marine environment (IAEA-SM-354/11P)... 309 R.C. Rastogi, K.-L. Sjoblom

Radioactive cesium, cobalt and plutonium in biota, algae and sediments in the

nonrestricted areas of the Russian Arctic Seas (IAEA-SM-354/12P)... 311 K. Rissanen, T.K. Ikaheimonen, D.G. Matishov, G.G. Matishov

Does benthic community structure influence radionuclide incorporation into the food web?

(IAEA-SM-354/15P)... 313 J. Carroll, S. Cochrane, M. Carroll, S. Dahle, M. losjpe, P. Strand

Peuplement des sables fins des cotes algeriennes: Amphipodes et pollution

(IAEA-SM-354/16P)... 315 A. Bakalem

2IOPo uptake by zooplankton during a one year cycle in relation to trophic conditions

in Monaco Bay (IAEA-SM-354/18P)... 318 J. Fdrber-Lorda, R.A. Jeffree, S. W. Fowler, F. Carvalho

Distribution of heavy metals in sediments of the Venice Lagoon: The role of the industrial

area (IAEA-SM-354/19P)... 320 M. Frignani, L. Giorgio Bellucci, M. Ravanelli, D. Paolucci

Reponse quantitative des communautes de nematodes soumises a 1'instabilite spatio-temporelle d'une lagune polluee: Le lac Sud de Tunis (IAEA-SM-354/20P)... 321 M. Hermi, P. Aissa

Modelling of I37Cs concentration change in organisms of the Japanese coastal food chains

(IAEA-SM-354/21P)... 323 Y. Tateda, M. Nakahara, R. Nakamura

The effects of s-triazines on selected marine microalgae (IAEA-SM-354/22P)... 325 S.A. Lewey, E.G. Nummela

Oxidative drug metabolizing enzymes in North Sea dab (Limanda limanda)

(biological effects of pollutants) (IAEA-SM-354/24P)... 328 M. Vobach, H.-J. Kellermann

Uptake and metabolism of 14C chlorpyrifos by marine bivalves (IAEA-SM-354/25P) ...330 C.-G. Zhong, S. Chen, X. Zhao, J. Shi, P.P. Carvalho

Numerical modeling of dispersion of pollutant in the coastal zone of the western Black Sea

(IAEA-SM-354/27P)... 332 P. Daniel, G. Mungov, G. Kortchev

Technogenic and natural radionuclides in Black Sea sediments and algae

(IAEA-SM-354/29P)... 334 A. Strezov, T. Stoilova, N. Petkov, M. Hristoskova

Modelling of migration of radionuclides and trace elements between the components

of the Black Sea ecosystems (IAEA-SM-354/3 IP)... 336 V.N. Egorov

Radiological background of the Georgian part of the Black Sea (IAEA-SM-354/33P)... 338 M. Avtandilashvili, A. Burchuladze, S. Pagava, Z. Robakidze, V. Rusetski, G. Togonidze

Damage to the testes of a marine fish, the plaice (Pleuronectes platessa), induced by chronic

exposure to low dose rate radiation (IAEA-SM-354/35P)... 340 J.F. Knowles

Assessment of heavy metals pollution in bottom sediments of the Arabian Gulf after the

Gulf War oil spill 1991 (IAEA-SM-354/36P)...342 S.M. Nasr, M.H. Ahmed, M. El-Raey, O.E. Frihy, A. Abdel Motti

Neutron-induced prompt gamma-ray analysis of Gulf marine environmental samples

(IAEA-SM-354/37P) „..„...„„...„„„„.„...„..„...„...„.„„....„„...„...„.„... 344 C. Yonezawa, H. Matsue, T. Adachi, M. Hoshi, E. Tachikawa, P.P. Povinec,

S. W. Fowler, M.S. Baxter

Determination of 237Np in sediments and seawater (IAEA-SM-354/38P)... 346

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Enhancement of 2IOPo and 210Pb arising from phosphate industry in the Syrian coast M.S. Al-Masri, S. Mamish, Y. Budeir

Natural and man-made radionuclide concentrations in marine sediments of Gokova Bay,

Aegean Turkish coast (IAEA-SM-354/41P) ... .350 A. U. Tanbay, G. Yener, S. Mulsow, S. W. Fowler, M. Duman

Heavy metal pollution in the sediments from the northern shelf of the Sea of Marmara

(IAEA-SM-354/42P)... ... ..352 O. Algan, N. Qagatay, N. Balkis, E. Sari, N. Kiratli, N. Gtingor, E. Gtingor

Biomagnification and bioaccumulation of mercury in two fish species from different trophic levels in the Bahia de Cartagena and the Cienaga Grande de Santa Marta,

Colombian Caribbean (IAEA-SM-354/44P) ... 354 D. Alonso, N. Campos

Study of bioaccumulation of mercury in shellfish (Tapes decussatus) from Tunisian coast

(IAEA-SM-354/45P) ... ....356 L Chouba, N. Zamouri-Langar, A. El Abed

Vertical fluxes of particulate metals in a northern Adriatic coastal area

(IAEA-SM-354/47P)... ... ..358 M. Giani, M. Gismondi, S. Righi, F. Savelli

Coral reefs and eutrophication (IAEA-SM-354/48P) ... 360 N. Stambler

Effects of heavy metals on the bioluminescence of the ophiuroid Amphipholis squamata:

A field study (IAEA-SM-354/50P) ... 362 D. Deheyn, M. Jangoux, M. Warnau

Marine radioactivity studies in the Suez Canal: Modelling hydrodynamics and dispersion

(IAEA-SM-354/52P)... ... .364 J.M. Abril, MM. Abdel-Aal

Influence of time and space resolution on dispersion of radionuclides and radioecological

assessment in the marine environment (IAEA-SM-354/54P) ... 366 M. Osjpe, P. Strand

Reconstruction and outlook of the radionuclide transport in the Mediterranean Seas chain

(IAEA-SM-354/55P)... ... ...368 V. Maderich

A radiological assessment of the nuclear reactors with spent fuel which have been scuttled in

the Kara Sea (IAEA-SM-354/58P) ... 370 S.P. Niels en, V. Maderich, V. Zheleznyak, L.M.C. Dutton, Y. Sivintsev, V. Lystsov,

E.I. Yefimov, T. Sazykina

Dispersion of radionuclides potentially released from the atolls of Mururoa and Fangataufa to neighbouring archipelagos (IAEA-SM-354/60P)... 372 /. Osvath

Predictions of radionuclide dispersion in seawater around the Mururoa and Fangataufa

atolls (IAEA-SM-354/61P) ... 374 O. Togawa

Plutonium-241 in seawater of the northwestern European Shelf Seas 1989-1993

(IAEA-SM-354/63P)... ... ...376 J. Herrmann, I. Goroncy

Caesium-137 in Baltic Sea sediments since the Chernobyl accident (1AEA-SM-354/64P) ... 379 E. Ilus, J. Mattila, H. Kankaanpda, A. Laine

239+24opu in settjjng particles on the East China Sea continental margin (IAEA-SM-354/65P) ... 381 M. Yamada, T. Aono

2iopo/2iopb disequiiibria in the Shelf edge of the East China Sea (IAEA-SM-354/66P) ... 383 T. Aono, M. Yamada, J. Zhang

Radium discharge due to oil off-shore production — case study: Bacia de Campos, Brazil

(IAEA-SM-354/67P)... ... .385 J.M. Godoy, N. Miekeley, S.F.J. Vegueria

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Preliminary results on laboratory simulations of the decomposition of the

green algae Ulva rigida (IAEA-SM-354/68P)... 387 S. Karavoltsos, M. Scouttos, H. Kaberi

The behaviour of 99Tc in UK waters 1995-1996 (IAEA-SM-354/69P)... 389 K.S. Leonard, D. McCubbin, H.S. Emerson, R.A. Bonfield

Origin and behaviour of radiocaesium, plutonium and americium in the sediment-water-biota

system of Strangford Lough (IAEA-SM-354/70P)... 391 P.I. Mitchell, R. W. Ryan, L. Lean Vintro, F.K. Ledgerwood, R.A. Larmour

Effet de la pollution sur la composition specifique et 1'abondance du zooplankton

dans les eaux cotieres syriennes (IAEA-SM-354/72P)... 393 M. Baker, H. Durgham

The fate of nutrients and phosphates in Akrotiri Bay, Cyprus Basin (eastern Mediterranean

Levantine Basin) (IAEA-SM-354/74P)... 395 G. Zodiatis, A. Demetropoulos, L. Loizides, M. Hadjichristoforou

Studies on plutonium and americium in coastal environment of Bombay Harbour Bay

(IAEA-SM-354/75P)... 397 V.M. Matkar, N. Us ha, K. Rudran

The IAEA '97 Pacific Ocean expedition (IAEA-SM-354/78P)... 399 P.P. Povinec, L. Htiynh-Ngoc, L. Liong Wee Kwong, S. Mulsow, B. Oregioni,

O. Togawa, I. Goroncy, H.H. Uhde, R. Rengarajan, K. Hirose, Y. Ikeuchi, T. Ito, S. Shima, M. Fukasawa, H. Moriya, T. Kazama, S. Ozawa, A. So, S. Yasuzumi, S.H. Lee, S.K. Park, H.B.L. Pettersson

Caprella watch: A new approach for monitoring butyltin residues in the ocean

(IAEA-SM-354/79P)... 401 /. Takeuchi, N. Miyazaki, S. Takahashi, S. Tanabe

Environmental pollutants in the Kara Sea and estuaries of Ob and Yenisey

(IAEA-SM-354/81P)...403 S. Dahle, A. Evenset, S. Cochrane, D. Loring, K. Nces

Environmental behaviour of pesticides in rice field drainage water. Impact on

the coastal zone (IAEA-SM-354/83P)... 405 G.F. Dierksmeier, P.L. Moreno, K. Martinez, R. Hernandez, C. Linares

Interaction between pesticides and humic substances from tropical coastal lagoons

(IAEA-SM-354/84P)...407 F. Gonzalez-Farias, P.P. Carvalho, S. W. Fowler, O. Cotret

Organochlorine residues in some dolphin specimens stranded on southern

Adriatic coasts (Italy) (IAEA-SM-354/85P)... 409 MM Storelli, R. Giacominelli Stuffier, E. Ceci, G.O. Marcotrigiano

Recent nordic intercomparison exercises on radioanalytical QA/QC (IAEA-SM-354/87P) 411 S.P. Nielsen, S.E. Palsson

Quality assurance programme for environmental radioactivity measurements at

the Hong Kong Observatory (IAEA-SM-354/91P)...„.„„„„.„..„.„...„...„„„.. 413 M.C. Wong,H.Y.Mok

Recent results in modeling Ge-gamma ray spectrometry measurements (IAEA-SM-354/92P)... 415 O. Sima

Development of an underwater Cherenkov detector to reveal sources of technogenic

radionuclides(IAEA-SM-354/93P)...417 AM. Chernyaev, LA. Gaponov, L. V. Lapushkina

Herbicides from the Charente river and the estuarine zone (Marennes-Oleron)

to the coastal seawater (IAEA-SM-354/94P)... 419 P. Scribe, S. Chouakri, S. Dupas, J.F. Dubernet

Intercomparison study of sampling methods for the determination of polychlorinated

biphenyl (PCB) in seawater (IAEA-SM-354/96P)... 421 D.E. Schulz-Bull

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Contaminants and nutrients in variable sea areas (CANVAS) — application of automatic

monitoring stations in the German marine environment (IAEA-SM-354/97P) 423 H. Nies, B. Brugge, D. Sterzenbach, H.D. Knauth, F. Schroder

Parametrisation and empirical model for bedload movement in the multibar coastal zone

on the base of field radiotracer study (IAEA-SM-354/98P)... ... 425 A. Owczarczyk, R. Wierzchnicki, Z. Pruszak

Accumulation of petroleum hydrocarbons in zooplankton of Banyas coastal waters (Syria)

(IAEA-SM-354/101P) ... 427 A.K. Youssef, H. Durgham, M. Baker, S. Noureddin

Vertical transport of suspended particulate trace elements in the north Atlantic Ocean

(IAEA-SM-354/103P). ... ....429 J. Kuss, K. Kremling, J. Scholten

Geochemical processes in the aquatic system on land and their influence on radionuclide

transfer to the oceans (IAEA-SM-354/104P)... 431 A. Albrecht, J. Beer, J-J. Geering, J-F. Valley

Chemocline chemistry (IAEA-SM-354/105P) ... 433 D. W. Dyrssen

Validation of a marine dispersion model for the calculation of doses to the European

population (IAEA-SM-354/107P) ... 435 T. Cabianca, A.P. Bexon

Information management system for environmental protection in the coastal area of Japan

(IAEA-SM-354/109P) ... 437 H. Hasegawa, T. Ajiro, N. Baba, Y. Michida, MTorigai

A comparison of doses from 137Cs and 210Po in surroundings of nuclear power plant

Juragua due to ingestion of marine food (IAEA-SM-354/1 1 IP) ... 440 CM Alonso Hernandez, R. Avila Moreno, M. Dias Asencio, A. Mimoz Caravaca,

E. Suarez Morell

Degradation, release and bioavailability of DDT/DDE residues to oysters using

radiolabelled techniques (IAEA-SM-354/1 16P) ... 442 CM Bajet, L.M. Varca, M.P. Navarro

River transport of radionuclides to the Arctic Seas, the Baltic Sea and the Black Sea

(IAEA-SM-354/118P) ... 444 M. Krosshavn, T. Nylen, G. Rusza, S.M. Vakulovsky, T. Walderhaug

Preventing pollution from US Navy ships (IAEA-SM-354/121P) ... 446 R. Bentley, V.E. Edgar

Distribution of some organochloride pesticides in the All Saints Bay, Bahia, Brazil

(IAEA-SM-354/122P) ... 448 M. Beretta, M.A. Costa, T.M. Tavares

Manganese kinetics in the shore crab Carcinus Maenas exposed via food and water

(IAEA-SM-354/123P) ... .450 P. Bjerregaard, M. Hastrup

Comparative bioaccumulation and toxicity of silver in different populations of the intra-sedimentary clam Macoma balthica exposed or not to metal contamination in

their natural medium (IAEA-SM-354/124P) ... 452 C. Amiard-Triquet, F. Boisson, C. Ballan-Dufrangais, B. Berthet, A. Geffard,

A-Y. Jeantet, C. Mouneyrac

Bioavailability of particles and low molecular mass species to the mussel Mytilus edulis P. B0rretzen, B. Salbu

Concentration des metaux lourds chez la palourde Ruditapes decussatus (L.) d'un milieu

lagunaire : le lac Mellah (el Kala) /Algerie (IAEA-SM-354/126P) ... 456 B. Boudjellal, W. Refes, B. Sellali, F. Ounadi, M. Azzouz, N. Eddalia, S. Benchikh

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Determination of radionuclides produced by Angra I nuclear power plant in marine samples collected in the bay "Saco de Piraquara de Fora" — Angra dos Reis City —

Rio de Janeiro (IAEA-SM-354/1 SOP)... 460 S.N.M. Cardoso, M.D.N. Santoro

The flow of radionuclides through the Canadian archipelago (IAEA-SM-3 54/134P)... 462 K. Ellis, J.N. Smith

Radiological study of Bardawill Lake in Egypt (IAEA-SM-354/135P)... 464 MS. El-Tahawy, A.E. Khater

Pu-239+240 and Pu-238 distribution among dissolved, colloidal and particulate phases

in the Rhone River (France) (IAEA-SM-354/137P)... ... 466 F. Eyrolle, F. Goutelard, D. Calmet

Marine pollution in Cameroon (Gulf of Guinea): State and remedies for successful

control and monitoring (IAEA-SM-354/138P)... 468 J. Folack

The Barents Sea, distribution and fate of radioactive contaminants (IAEA-SM-354/139P)... 471 L. F0yn, H.E. Heldal, I. Sv&ren

Produced water from off-shore oil and gas production, a new challenge in marine pollution

monitoring (IAEA-SM-354/140P)... 474 L. F0yn

Assessment of the Adriatic sea-water mean residence time using fallout 90Sr as radioactive

tracer (IAEA-SM-3 54/14 IP)...477 Z. Franic

History of mercury migration from Minamata Bay to the Yatsushiro Sea— the beginning of the migration, effect of reclamation and recent tendency

(IAEA-SM-354/142P)...479 Y. Fujikawa, H. Takigami, A. Kudo, M. Mitui, M. Sugahara, S. Miyahara,

T. Muramutsu

Global marine radioactivity database (GLOMARD) (IAEA-SM-354/143P)... 481 P.P. Povinec, J. Gayol, O. Togawa

Uptake and release of 65Zn and I24Sb on Biomphalaria Alexandrina and Cleopatra Bulimoides snails and their effects on the ultrastructure of the

hermaphrodite gland (IAEA-SM-354/147P)... 483 H. Moloukhia, A. Allan

Aliphatic hydrocarbons and hopanes as biomarkers of the past 120 years sediment

inputs in a coral reef lagoon (Tahiti, French Polynesia) (IAEA-SM-3 54/148P)... 485 P.A. Harris, R. Fichez, J-M. Fernandez, A. Saliot

Organotins and osmoregulation: Quantifying the effects on the European flounder

PlatichthysJlesus(IAEA-SM-354/l49?)...487 M.G.J. Hartl, S. Hutchinson, L.E. Hawking

Biogeochemical studies of selenium in the Indian Ocean (IAEA-SM-3 54/1 SOP) 489 H. Hattori, Y. Nakaguchi, K. Hiraki, M. Kimura, Y. Koike

Polycyclic aromatic hydrocarbons (PAH) in seawater from the northern Aegean Sea,

Greece (IAEA-SM-354/151P)... 491 J. Hatzianestis, E. Sklivagou, V. Zervakis, D. Georgopoulos

Specific accumulation of iodine by the operculum of the strawberry conch Strombus

/w/ma«Hs(IAEA-SM-354/155P)... 493 T. Ishii, T. Miyazaki, M. Nakahara, R. Nakamura, T. Watabe

AMS measurement of 36C1,129I and 14C in waters from Mururoa and Fangataufa Atolls

(IAEA-SM-354/156P) ... 495 G.E. Jacobsen, M.A.C. Hotchkis, D. Fink, D. Levins, D.P. Child, C. Tuniz, E. Sacchi

Radiocaesium in Fucus vesiculosis along the Swedish coast between 1986-1995

(IAEA-SM-354/158P)...497 E. Holm, D. Josefsson, P. Roos, M. Eriksson

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Development of a submersible Ge gamma-ray detector system (IAEA-SM-354/161P) 501 Y. Kobayashi, R. Takahashi, S. Shima, M. Katagiri, K. Takahashi

A preliminary investigation on the pollutant distribution in the south eastern Black Sea

coast (IAEA-SM-354/162P)... 503 E. Kose, B. Sonaiez, S. Ozcoban, F. Ozer, C. Erliz, K. Seyhan, A.C. Dincer, Y. Malkoc

Trace metal concentrations in marine organisms from the eastern Aegean, Turkey

(IAEA-SM-354/163P) ...„...„„„.„..„„.„„...„.„„„... 506 F. Kucuksezgin

Radiocaesium, plutonium and americium partitioning and solid speciation in sized,

inter-tidal sediments from Strangford Lough (IAEA-SM-354/164P)... 509 F.K. Ledgerwood, R.A. Larmour, P.I. Mitchell, L Lean Vintro, R. W. Ryan

An operational oil spill model for the Levantine Basin (eastern Mediterranean Sea)

(IAEA-SM-354/166P) ... 511 R. W. Lardner, G. Zodiatis, L. Loizides, A. Demetropoulos

The activity and the development of radioecology marine laboratory in Indonesia

(IAEA-SM-354/167P)... 513 E. Lubis, H. Umbara, S. Yarbaini, G. Unandjar

The red alga Gracilaria verrucosa (Huds.) Papens. as an indicator for metal pollution in

Thermaikos Gulf (Greece) (IAEA-SM-354/169P)... 515 P. Malea, S. Haritonidis, T. Kevrekidis

Time dependent phase associations of iron and other trace elements elucidated by

234Th/238U inventories in tropical coastal waters (IAEA-SM-354/171P)... 517 R. Szymczak, M. Zaw

Impact of a coal fired power plant on 226Ra activity level in sea water

(IAEA-SM-354/172P)... 519 G. Marovic, J. Sencar

Environmental impact of the minero-metallurgic industry on the marine ecosystem in Moa,

Cuba (TAEA-SM-354/173P)... 521 M. Martinez Canals, L. Pedro Garcia

Distribution of I29I: Evidence for world-wide influence of nuclear fuel reprocessing

(IAEA-SM-354/174P)... 524 U. Fehn, G. Snyder, J.E. Moron

Geographic and vertical distribution of global fallout americium 241, plutonium isotopes

and cesium 137 in lake sediments (IAEA-SM-354/177P)... 526 H. Michel, G. Barci-Funel, J. Dalmasso, G. Ardisson

Using stable carbon and nitrogen isotope ratios for understanding trophic structure in the

Seto Inland Sea, Japan (IAEA-SM-354/178P)... 528 Y. Mishima, A. Hoshika, T. Tanimoto, S. Uye

Results and analysis of the Amara sea water intercomparison for 137Cs, 238Pu and

239'240Pu(IAEA-SM-354/179P)... 530 P.I. Mitchell, E. Holm, H. Dahlgaard, S.P. Nielsen, D. Boust, K.S. Leonard,

C. Papucci,B. Salbu, P. Strand, J.A. Sanchez-Cabeza, K. Rissanen, D. Pollard, C. Gasco, G.C. Christensen, L. Lean Vintro, C.A. McMahon, J. Herrmann, H. Nies Distribution and transfer of dissolved trace metals in the north Aegean Sea

(IAEA-SM-354/181P)... 532 A. Moriki, C. Zeri, V. Zervakis, D. Georgopoulos

Coprecipitate mechanism of trace elements in coastal environment formation and structure

of plural hydroxide (IAEA-SM-354/184P)... 534 T. Nishimura, Y. Nakaguchi, Y. Suzuki, K. Hiraki

Applications of artificial radiotracers in studies of sediment and contaminant transport in the

coastal zone (IAEA-SM-354/185P)... 536 R. Szymczak, P. Airey, J.Y. Tu

Radioactivity of some alpha, beta and gamma emitting radionuclides in surface marine

sediments of different bays in Algeria (IAEA-SM-354/186P)... 538 A. Noureddine, B. Baggoura

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Distribution of 137Cs in surface and deep water in the central part of Algerian littoral

(IAEA-SM-354/187P)...„...„....„.„..„„„„„...„..„...„....„.„....„... 540 A. Gheddou, A. Noureddine, M. Menacer, R. Boudjenoun, A. Hammadi, M. Benkrid,

A. Bourezak

Distribution of 137Cs in sediments in Xiangshan, Xiamen and Yangpu harbours, China

(IAEA-SM-354/191P)... 542 S.Pan, Q.Xu

Transfer! des radionucleides 60Co, 65Zn et 134Cs aux sediments et aux mollusques

marins en conditions de laboratoire (IAEA-SM-354/I93P)... 544 V. Patrascu

Techniques nucleaires et resultats du monitoring roumain de la Mer Noire dans le Laboratoire Radioecologique de 1'Institut Roumain de Recherches

Marines (IAEA-SM-354/194P) ..„....„...„„„...546 V. Patrascu

Monte Carlo modelling of the dispersion of radionuclides from the Mururoa test site

(IAEA-SM-354/195P)... 548 J. Masarik, P.P. Povinec

Radioactive contamination of the Guatemalan marine environment (IAEA-SM-354/197P) 550 J.F. Perez-Sabino, B.E. Oliva de Sandoval, R.M. Orozco-Chilel, E. Aguilar-Sandoval

Distribution of particulate trace metals along Visakhapatnam coast (Bay of Bengal)

(IAEA-SM-354/199P)... 553 D. Satyanarayana, P. V.S. Prabhakara Murty

Natural and artificial radionuclides in southern Gulf of Mexico marine sediments

(IAEA-SM-354/203P)... 555 P.P. Rodriguez-Espinosa, V.M. V. Vidal-Lorandi, F. V. Vidal- Lorandi

Time-trend in the deposition of Sellafield derived plutonium in the northeastern

Skagerrak high sediment accumulation rate area (IAEA-SM-354/204P) ...557 P. Roos, E. Holm, P. Hall

Modelling receiving water quality responses to brackishwater shrimp aquaculture farm effluents (IAEA-SM-354/205P)... 559 R.K. Roy Chaudhury, V, Ramana Murty, M. Ravindran

Contexte mediterraneen de la circulation des eaux le long des cotes tunisiennes

(IAEA-SM-354/209P)... 561 C. Sammari

Distribution of aliphatic and aromatic hydrocarbon in dated sediment cores of the Gulf of

Thailand (IAEA-SM-354/210P) ... 563 C. Sarin, K. Srisuksawad

Release and transport of artificial radionuclides from nuclear weapons related activities

in the Ob River, Siberia over the course of the nuclear age (IAEA-SM-354/21 IP) 565 F.L Sayles, T.C. Kenna, H.D. Livingston

Radiocaesium-137 in some marine species in coastal zone of Libya (Sirt Gulf)

(IAEA-SM-354/213P)... 568 M.A. Shenber, E.E. Elshamis, A.T. Elkikli, M.N. Elayan

Radionuclides and heavy metals as tracers of the eastern Black Sea contamination history

(IAEA-SM-354/214P)... 570 KM. Shimkus, J.M. Grebmeier, L. W. Cooper

Dynamics of distribution coefficients in estuarine systems (IAEA-SM-354/216P)... 572 M. Sickel, P. B0rretzen, B. Salbu

Trace metals in Mediterranean mussel Mytilus galloprovincialis (L.I758) and in

surficial sediments from Urla-Yskele/Turkey (IAEA-SM-354/22IP)... 573 U. Sunlit, 6. Egemen, A. Kaymakty

Distribution of pollutants in the Russian sector of the Black Sea coastal zone

(IAEA-SM-354/222P)... 576

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Effect of environmental conditions on Cs-137 accumulations in Japanese seabass

(LateolabraxJaponicus)(IAEA-SM-354/224P)... 578 Y. Suzuki, Y. Ishikawa, F. Kasamatsu, Y. Nagaya, S. Sakamoto, M Nakahara,

R Nakamura

Effect of terrestrial fluorescent substances on dissolved organic matter in the coastal

environment (IAEA-SM-354/225P)... 580 Y. Suzuki, Y. Nakaguchi, T. Nishimura, E. Kawakami, K. Hiraki, M Aihara

A survey of marine and aquatic oil spills in the Philippines from 1975-1997

(IAEA-SM-354/227P)... 582 T.P.N. Talorete

A biomonitoring program of the coastal area of the Principality of Monaco

(IAEA-SM-354/228P)... 584 S. Tambutte, E. Tambutte, P. Rolland, M-C. van Klaveren

Radiotracer studies on radionuclide and trace element cycling in corals

(IAEA-SM-354/230P)...587 S. W. Fowler, J-L Teyssie, A. Acosta, J-P. Gattuso, J. Jaubert

Influence of food quality on the assimilation, retention and distribution of selected trace elements and radionuclides in the Mediterranean crab Pachygrapsus

warmo/ato (IAEA-SM-354/23IP)... 589 J-L. Teyssie, S. W. Fowler, G. Schonbeck

Hazardous chemicals in marine mammals from the western North Pacific

(IAEA-SM-354/232P) ...„„„...„.„.„...„.„...„„...„....„..„.„....„....„.„„...591 N. Miyazaki, S. Tanabe, R. Tatsukawa

A survey of heavy metals in mussels (Monaco, 1989-1996) (IAEA-SM-3 54/23 7P)... 593 A. Veglia

Monte Carlo modelling of background characteristics of HPGe detectors for marine

radioactivity measurements (IAEA-SM-354/238P)... 595 P. Vojtyla, P.P. Povinec, C. Dovlete

Trace elements, pesticides and PCBs levels in sediments of a bay influenced by

anthropogenic activities (Thermaikos Bay, N.W. Aegean Sea) (IAEA-SM-354/239P)... 597 .P. Voutsinou-Taliadouri, J. Hatzianestis, E. Georgakopoulou-Gregoriadou

Uptake and loss of heavy metals and radionuclides in the common NE Atlantic starfish

Asterias rubens: Seawater and food exposures (IAEA-SM-354/240P)... 599 M. Warnau, S. W. Fowler, J-L. Teyssie

The fate of 137Cs in the coastal seas of Japan and resultant dose from intake through

fishery products (IAEA-SM-354/24IP)... 601 T. Watabe, T. Miyazaki, M. Matsuba, S. Yokosuka

Occurrence of chlorinated pesticides in mussels of Guanabara Bay, Rio de Janeiro, Brazil

(IAEA-SM-354/242P)... 603 A.P. Xavier de Brito, I.M.R. de Andrade Bruning, I. Moreira, I. Loureiro

Changes in marine fish community under influence of Leningrad Nuclear Power Plant and other human activities in the watershed of Koporskaya Bay

(Gulf of Finland, Baltic Sea) (IAEA-SM-354/247P)... 605 V.L. Zimin

The fate of nutrients and phosphates in Akrotiri Bay, Cyprus Basin (eastern Mediterranean

Levantine Basin) (IAEA-SM-354/248P)... 607 G. Zodiatis, A. Demetropoulos, L. Loizides, M. Hadjichristoforou

Distribution of Cs-137 and Pu-239+240 in marine sediments from Brazilian southern coast

(IAEA-SM-354/250P)...„..„...„....„„„„..„.„.„„...„...;...„....„...„...„ 609 R.C.L. Figueira, ILL. Cunha, V.V. Furtado

Present and potential contamination of the river system at Mayak "PA"

(IAEA-SM-354/254P)... 612 /. Amundsen, P. Strand, S. V. Malyshev, E.G. Drozhko, G.N. Romanov, Y. V. Glagolenko,

Y.G. Mokrov, B. Salbu, D.HOughton, G. Christensen, T.D.S. Bergan

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Organochlorine residues in sediments from selected tributaries to Manila Bay, Philippines

(IAEA-SM-354/255P) ... ... 614 C.M. Bajet, L.M. Varca, M.P. Navarro

Avoiding pollution in scientific ocean drilling (IAEA-SM-354/258P). ... 616 T-J.G. Francis

Euro Chlor risk assessment for the marine environment Osparcom region — North Sea

(IAEA-SM-354/259P)...618 V. Garny, J-C. Boutonnet, A. Lecloux, R. Papp, C. de Rooij,

R.S. Thompson, D. Van Wijk

Plutonium and polonium concentrations in the different water masses crossing

the Strait of Gibraltar (IAEA-SM-354/260P)... ... 620 C. Gasco, M.P. Anton

Transport of radionuclides in the Kara Sea and eastern Barents Sea (IAEA-SM-3 54/26 IP) 622 M. Krosshavn, T. Eng0y, J. Can-oil, D. Johnson, S.E. King, P. Varskog

The flux of particles and contaminants in the Skagerrak (IAEA-SM-3 54/263 P) ... 624 T. Noji, C. Noji, LA. Miller, J. Klungs0yr, L. F0yn

The lessons learnt from a series of radioactivity measurement intercomparison

exercises (IAEA-SM-3 54/264P) ... ..626 S.M. Jerome, M.J. Woods

Dynamics of particle sedimentation in the open NW Mediterranean Sea

(IAEA-SM-3 54/266P) . ... 627 J-C. Miquel, S. W. Fowler, J. La Rosa, L. Stemmann, J. Chiaverini, Y. Chaabeni,

J-C. Marty

Artificial radioactivity in Carlingford Lough, Ireland (IAEA-SM-3 54/270P)... ... 629 S. Long, E. Hoyden, V. Smith, M. Fegan, A. Dowdall, D. Pollard, R. Larmour,

K. Ledgerwood, L. Peake

Characterization, impact and fate of atmospheric inputs in the water column V. Sandroni, C. Migon

Assessment of the risk created by the objects with spent nuclear fuel dumped in

the Kara Sea and instrumental possibilities of the early warning about radionuclides

discharges from these objects (IAEA-SM-3 54/276P) ... 634 V. Lystsov, N. Mwzin, G. Nezhdanov

Long range transport of hydrocarbons in the southern ocean (IAEA-SM-354/277P) 636 L. Pinturier, J. Laureillard, M. Arnold, N. Tisnerat, J-J. Pichon, J. Gireaudau

Alterations in the organic carbon pool recorded in sediments of Guanabara Bay, Brazil,

a fertilized tropical estuary (IAEA-SM-354/278P) ... 638 R.S. Carreira, F.A. Kalas, E.S. Santos, A.L. Lima, J.M. Godoy, A.L.R. Wagener

Monitoring and measurements of radioactivity around the valley of Madjerdah River

in Tunisia (IAEA-SM-354/279P) ... 640 N. Reguigui, H, Ben Kraiem, H. Latrons

Pb, Cd, Cu and Zn biogeochemical behaviour and biological transfer processes in the

northwestern Mediterranean (IAEA-SM-3 54/280P) ... 644 E. Nicolas, J-C. Marty, J-C. Miquel, S.W. Fowler

The DYFAMED time-series station: A reference site for environmental studies in the north

western Mediterranean Sea (IAEA-SM-3 54/28 IP) ... 646 J-C. Marty, I. Vescovali, K. Oubelkheir, A. Stock, J. Chiaverini, M-D. Pizay

Monitoring of radionuclides in the air of Monaco during 1997-1998

(IAEA-SM-354/282P) ... 648 M.K. Pham, P.P. Povinec, L. Huynh-Ngoc

Assessment of algeciras fallout distribution over the southern part of France

(IAEA-SM-354/283P) ... ... 650 D. Calmet, E. Barker, J.P. Melquiond, P. Cedrola, P. Bouisset, O. Masson, M. Arnaud,

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Marine radioactivity measurements with liquid scintillation spectrometers

(IAEA-SM-354/285P)... 652

L Liong Wee Kwong, P.P. Povinec Chairmen of Sessions... 655

Secretariat of the Symposium ... 656

List of Participants.. ... 657

Index of Paper Numbers by Thematic Area... 692

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IAEA-SM-354/7 TEMPORAL VARIATIONS IN PLUTONIUM AND AMERICIUM INVENTORIES IN THE NORTHWESTERN MEDITERRANEAN SEA AND THEIR RELATION TO VERTICAL PARTICULATE FLUX

FOWLER, S.W., V.E. NOSHKIN*, J. LA ROSA, J. GASTAUD XA9951888 International Atomic Energy Agency

Marine Environment Laboratory, Monaco

Abstract

Temporal changes in 239+240pu and 241Am inventories in the western Mediterranean have been examined by making high resolution water column sampling and direct measurements of the vertical flux of particle-bound transuranics using time-series sediment traps. Water column profiles of both radionuclides showed well-defined sub-surface maxima (239+240pu between 100-400 m; ^'Am at 100- 200 rn and 800 m). Time-series measurements of 239+240pu indicated a shift in the depth of the sub- surface maxima which appeared to be related to a change in depth of the core of low-salinity Levantine Intermediate Water. Total water column inventories for the western basin compared with total fallout inventories for the same area show that by 1990, approximately 56% of the 239+240pu and 20% of the 241 Am deposited in the basin still resided in the water column. Time-series measurements of the downward flux of paniculate 239+240pu and ^Am compared with transuranic removal rates derived from observed total water column inventory differences over time, show that particles sinking out of deep waters (1000-2000 m) could account for 26-72% of the computed total annual 239+240pu

loss and virtually all of the 241 Am removal from the water column. Computed upper water column (0- 200) residence times were 20-30 y for 239+240pu and 5-10 y for M1Am in the open waters of the northwestern Mediterranean. A comparison with data for the north Pacific Ocean indicate that 239+240pu residence times are shorter and those for 241Am much longer in open waters of the northeast Pacific. 241Am/239+240Pu activity ratios in unfiltered sea water from the western Mediterranean which are six times lower than those in the north Pacific indicate the existence of a mechanism for enhanced scavenging and removal of ^Am from Mediterranean waters. It is proposed that frequent atmospheric inputs of aluminosilicate particles transported by Saharan dust events could enhance geochemical scavenging and removal of ulAm to the sediments of the western Mediterranean basin.

1. INTRODUCTION

One of the main objectives of oceanic flux studies is to examine spatial and temporal variability of the downward vertical transport of key elements and radionuclides involved in marine biogeochemical cycles. Two long-lived transuranic elements, plutonium and americium, have entered the marine environment as contaminants primarily via fallout from atmospheric weapons testing. The different chemical behaviours of these artificial radionuclides in sea water have made them unique tools for studying various particle-related processes in the ocean [1-4].

As a result of increasing interest in such anthropogenic tracers, a substantial database has accrued on the distribution and behaviour of plutonium and americium in sea water, suspended particulates and sediments. However, direct measurements of the particle-associated vertical flux of plutonium and americium remain rare, even though such information is essential for quantifying their residence times and removal rates in the water column [3-5]. Another method for deriving the downward

^Present address: Lawrence Livermore National Laboratory, Univ. of California, Livermore, CA 94550, USA

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movements of surface-introduced transuranic elements is to compare sea water radionuclide inventories for given depth intervals over different periods of time. Based solely on sea water profiles measured in the mid-1970s and early 1980s, it has been postulated that the association of transuranics with sinking particles is responsible for the slow downward displacement of dissolved plutonium and americium reported for Mediterranean waters [2]. In order to refine such critical comparisons, we have measured high resolution depth profiles of plutonium and americium in the northwestern Mediterranean basin during a series of cruises in 1989-90. The profiles were taken at two offshore stations where time-series sediment trap experiments were also underway to quantify the present downward vertical flux of transuranium nuclides and other elements.

2. METHODS AND MATERIALS 2.1 Sea water profiles

Unfiltered sea water samples were collected during three separate cruises at two locations in the northwestern Mediterranean basin. During May and November 1989, two sampling cruises were undertaken at the French DYFAMED station (43°25'N, 07°53'E) located approximately 30 nautical miles southeast of Cap Ferrat, France. On each occasion sea water was collected at 17 depths by casts employing 30 1 Niskin bottles mounted on a Rosette sampler. Approximately 60 1 of sea water was taken at each depth to a maximum depth of 2250 m. In May 1990 during the 'CYBELLE' cruise, 19 depths were sampled by taking similar casts down to a depth of 2470 m at the EROS-2000 'ETRO' station (41°57'N, 05°56'E) in the Gulf of Lions approximately 60 nautical miles south of Toulon, France.

2.2 Particle fluxes

Automated time-series sediment traps were used to collect sinking particles at both stations during various periods between June 1988 and July 1990. At the DYFAMED station from June 1988 to December 1989, traps moored at 100, 200, 1000 and 2000 m collected material for time intervals ranging from 14 to 27 days. In spring-summer of 1990 sediment traps were moored at the EROS 2000 'ETRO' station in the Gulf of Lions at depths of 200, 500, 1000 and 2000 m. Each of the six collection cups sampled a consecutive 13-day period between 14 April and 1 July 1990. Trap design, sample preservation methodology and protocols for treatment and preparation of the paniculate samples are described in detail elsewhere [7].

2.3 Radionuclide analysis

Unfiltered sea water samples were acidified with HNO3 to pH 1, spiked with appropriate yield determinants (M2Pu and 243Am), and the transuranium nuclides carried down by an Fe(OH)3

precipitation. The precipitate was subsequently dissolved and 239+240pu and 241Am chemically separated and purified by methodologies described previously [1,6]

Freeze-dried particulate samples from the sediment traps (20-110 mg dry) were ground to a fine powder in an agate mortar. Aliquots were then spiked with yield determinants, digested in a concentrated HNO3-HC1O4 mixture and evaporated to dryness. Any siliceous residue remaining after the initial dissolution was further treated with HF until a clear solution was obtained. All samples were subsequently taken to dryness, brought to volume with dilute HNO3 and co-precipitated with Fe(OH)3. The separated and purified 239+240pu and 241Am from the particulates were electrodeposited onto stainless steel discs and measured by alpha spectrometry using silicon barrier detectors.

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3. RESULTS AND DISCUSSION

3.1 Transuranium profiles and inventories

Concentration profiles for the radionuclides are shown along with the 241Am/239+240Pu activity ratios in Figure 1. All three high resolution profiles of 239+240pu show a distinct sub-surface maximum in concentration. The DYFAMED Nov. 1989 and EROS plutonium profiles are quite similar in shape with sub-surface maxima evident between 100-400 m. The May 1989 profile at the DYFAMED site was somewhat different from that taken at the same station six months later in that during May the sharp sub-surface maximum was centered at 100 m, whereas in November 1989 it had shifted to a depth of 400 m. The sub-surface plutonium maximum in November was observed at the same depth as the salinity maximum (38.57 PSU; Fig. 1) which closely reflects the depth of the core of Levantine Intermediate Water in this region. During May of the same year, the salinity at 100 m (38.49 PSU; Fig. 1) was much higher than that measured during November (38.13 PSU) and most likely was responsible for the maximum 239+240pu levels observed at the same depth in May. This feature, which has been observed previously, is generally attributed to the downward vertical transport and subsequent mineralization of plutonium-enriched organic particulates which release the radionuclide back into the water column. While such a biogeochemical mechanism is probably of primary importance in maintaining the presence of this feature in the upper water column, the temporal data from the DYFAMED station indicate that hydrodynamic changes in water mass distribution in the northwestern Mediterranean may influence its exact positioning in the upper 400 m.

The ^'Am profile shows two sub-surface maxima, a smaller one between 100-200 m that corresponds to the Pu sub-surface maximum and a much sharper maximum centered at 800 m depth (Fig. 1). The significance of the deep sub-surface maximum is not clear but may be related to enhanced scavenging of 241Am by particles at this depth; however, whatever the process involved, it does not affect the corresponding vertical distribution of 239+240Pu.

Interpretation of these profiles would be greatly facilitated by knowledge of how the concentrations have changed at various depths in the water column over time. To do this, historical data prior to 1989 from the entire western Mediterranean were assembled and inventories for various depth intervals computed. Most of the earlier profiles were comprised of very few sampling depths, which limits the accuracy of determining water column inventories; therefore, only two deep water column profiles, which were taken very near our 1989-90 stations and included at least 7 sample depths, were selected for purposes of detailed inventory comparisons.

The 239+240pu inventories based on measurements made to at least a depth of 2000 m show that very little decrease in total inventory (~2 Bq m"2) had occurred during roughly the decade over which the measurements were made. However, 239+240pu inventories in the lower 1000-2000 m depth interval of the 2000 m water column have clearly increased over that time interval. Computations indicate whereas in the 1976-82 time frame only 33% of the 239+240pu water column inventory resided within the lower 1000 m depth interval, by 1989-90 the percentage had increased to 46%. With the increase in deep water plutonium inventories, there was a concomitant decrease of approximately 35% in the upper mixed layer (0-200 m) during this time. These data show that plutonium is slowly being removed from the surface layers and accumulating in the deeper waters of the western Mediterranean.

Inventories in different depth intervals were constructed and compared with a detailed 241Am profile taken in the northwestern basin nearly 14 years earlier [1]. The data show that the depth distributions of 241Am are more complex than those of plutonium. Except in the upper mixed layer (0-200 m), there has been a clear decrease in the inventories over time. The entire 2000 m water column inventories indicate that there was roughly a 24% decrease in 241Am during the period 1976-

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90. Nevertheless, the fraction of that inventory residing in the deeper 1000-2000 m depth interval was the same (-56%) at both times. Thus, whereas 239+240pu has shown a slow increase in the amount retained in the lower half of the 2000 m water column over this time period, the corresponding 24!Am data suggest a rapid transfer from the water column, most probably into the sediments.

These transuranic inventories deal only with the measured concentrations within the upper 2000 m of the water column in the western Mediterranean. However, nearly one half of the surface area of this region is represented by depths greater than 2000 [8], thus, any realistic computation of total transuranic inventories for the western Mediterranean must include inventories for these depths. In order to estimate inventories at depths greater than 2000 m, the cumulative inventories for 239+240pu

and 241Am at each station were plotted and were found to increase linearly with depth; therefore, inventories below this depth were derived by extrapolation of this relationship.

239+240pu inven£0rjes to depth were determined in this fashion for three separate time periods, i.e.

1976, 1981-82 and 1989-90. The cumulative inventories in different depth intervals were then multiplied by the areas of those depth intervals in the western Mediterranean basin to arrive at estimates of the total water column transuranic inventory for each time period. In the case of ^'Am, profile data for the western basin are fewer, hence, a comparison of total water column inventories has only been made using the measured inventories from only two stations. The differences in total water column inventories of 239+240pu and ^'Am over time and the computed mean annual loss of these radionuclides from the water column are given in Table 1. From this assessment it is evident that a greater fraction of the 24lAm inventory has been removed from the water column over the years than for 239+240Pu.

From known deposition rates in the northern hemisphere and observed 241Am/239+240Pu ratios in soil samples [9,10], it can be calculated that total integrated 239+240pu and 241Am delivery by 1990 was 54.3 and 20.1 TBq, respectively. Comparing the total water column inventories for 1989-90 with the total delivery values indicates that 56% and 20% of the deposited 239+240pu and ^Am, respectively, were still present in the water column at that time.

3.2 Vertical Fluxes

Concentration of both radionuclides in the sinking particulate matter were similar at the two stations ranging from approximately 0.3 to 8 Bq kg"1. The 24!Am/239'f240Pu ratios in the particles were all higher than were observed in bulk sea water, and some very high ratios (1.9 - 2.4), more typical of Mediterranean sediments [11] were recorded in particles fluxing through 2000 m.

During the course of the 2Vz month EROS experiment from April to July, the 239+240pu

concentrations in particles at 200 m steadily increased from 1.92 - 8.45 Bq kg"1. Corresponding

241 Am levels varied by a factor of 10 throughout this period but did not follow the same increasing trend as 239+240Pu. Both 241Am concentration and flux increased with depth suggesting enhanced scavenging of the radionuclide throughout the water column. Preferential scavenging of 24!Am relative to 239-i'240pu is aiso reflected in the increasing 241Am/239+240Pu ratio in the sinking particles with depth. The maximum fluxes of both 239+240pu and ^Am coincided with the period of maximum sedimentation indicating that mass flux was the main factor controlling transuranic flux. These fluxes measured at both stations were similar to those recorded in the same region off Corsica during spring 1986 [3] but they were an order of magnitude lower than 239+240pu and 241Am fluxes measured in the high sedimentation regime of the Lacaze-Duthiers Canyon in the Gulf of Lions [4]. Clearly, variations in the flux of these radionuclides largely depend on the sedimentation rate.

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DYFAMED, MAY 1989 mBq m"

10 20 30 40 50

Depth (m)

DYFAMED, NOV. 1989 mBq m""' 10 20 30

DePth1500 (m)

40

EROS 2000, ETR-0 Station mBq m"

0 10 20 30 40 50 0 1

EROS 2000, ETR-0 Station mBq m"

2 3 4

Depth

EROS 2000, ETR-0 Station (Am/Pu activity ratio)

0.0 0.1 0.2 0.3 0.4 0.5

Depth (m)

SALINITY (psu)

38.00 38.20 38.40 38.60 38.80

500 • 05/1990 1000 - • 5/1989

Depth

FIG. 1. Vertical profiles of239+240Pu (DYFAMED & EROS 2000 stations), 24!Am (EROS 2000) and

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The degree to which large particle transport is responsible for the removal of 239+240pu and 241Am from the water column can be examined by comparing measurements of mean annual transuranic fluxes, particularly those in deep waters, with the estimates of changes in total water column plutonium and americium inventories over time (Table 1). Comparing these deep water (1000-2000 m) paniculate transuranic fluxes in the open waters of the western basin (0.10 - 0.28 for 239+240Pu;

0.10 - 0.22 for ^Am) with the derived annual loss rates suggests that from 26-72% of the estimated plutonium loss can be accounted for by the sinking out of large particles, whereas virtually all of the

241 Am removed could have occurred by this mechanism.

TABLE I. SUMMARY OF WATER COLUMN INVENTORIES (TBq) FOR TRANSURANICS IN THE WESTERN MEDITERRANEAN SEA AND MEAN ANNUAL TRANSURANIC LOSS (Bq m V') DERIVED FOR DIFFERENT TIME INTERVALS

____ ___

Inventory for years

1976 (T,) 198 1-82 (T2) 1989-90 (T3)

34.1 TBq 33.2 TBq 30.3 TBq

5. 19 TBq 3.95 TBq Inventory decrease

between years

T2-Tj 0.9 TBq

T3-T2 2.9 TBq

T3-T, 3.8 TBq 1.24 TBq

*Mean loss per year for different time intervals

T2-T, 0.24 Bq m'V1

T3-T2 0.53 Bq m V1

TS-T, 0.41 Bq m'V ____ O.BBqm'V Overall mean loss ___________________ 0.39 Bq m'V ____ O.lSBqm'V1

The difference in inventories between any two-year intervals is computed as the inventory decrease divided by the total surface area of the western Mediterranean basin (681xl09m2) divided by the average time interval between the years when measurements were made (i.e. 5.5, 8 or 13.5 years).

The average 239+240pu and ^'Am flux through 200 m during the two-and-a-half month EROS- 2000 study was 0.688 and 0.273 mBq m'M"1, respectively. Transuranic concentration profiles in sea water measured at this site during early May resulted in corresponding radionuclide inventories above 200 m of 5.9 and 0.53 Bq m"2. Such fluxes would result in a residence time for 239+240pu anci 241 Am in the upper mixed layers of approximately 24 and 5.3 y, respectively. These residence times are considerably longer than those (2.5 and 0.14 y, respectively) reported for a 17-day deployment in the Lacaze-Duthiers Canyon [4] and are therefore more representative of average transuranic flux in open waters of the northwestern Mediterranean. Mean upper layer (0-200 m) residence times of 239+240pu

and 241Am have been computed for various areas in the northwestern Mediterranean and were found to be approximately 5-10 years for ^Am and 20-30 years for 239+240Pu.

Comparison of transuranic residence times in the Mediterranean with those derived from north Pacific Ocean data shows that the residence times for 239+240pu in the Pacific were shorter than those measured at the open Mediterranean stations. Comparable data for ^'Am are fewer; nevertheless, in oligotrophic waters of the north Pacific gyre station, the ^Am residence time (37 y) is roughly twice as long as that of 239+240pu which is the opposite of that observed in the western Mediterranean. Thus, it appears that the biogeochemical behaviour of these fallout radionuclides in the upper water column of oligotrophic waters from these two open ocean regions is quite different. An examination of

24IAm/239+240Pu ratios measured in a variety of unfiltered sea water samples from the two oceans

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demonstrates that ratios in western Mediterranean waters are on average some six times lower than those in the north Pacific. Such a large impoverishment of ^Am relative to 239+240pu in Mediterranean sea water points to a mechanism for effecting much more rapid removal of 241 Am from Mediterranean waters. It is proposed that the frequent atmospheric inputs of massive amounts of aluminosilicate particles to the Mediterranean via Saharan dust storms furnishes a particle type for which ^'Am has a greater binding affinity than 239+240pu which, in turn, leads to higher vertical transport rates relative to 239+240pu jn the Mediterranean, and higher 241Am transport in general compared to that in the open north Pacific.

Acknowledgements

This work was supported in part by the French JGOFS Programme "DYFAMED", and the CEC Marine Science and Technology Programme under contract MAST-0016-C (EBD) as part of the EROS-2000 project. We thank the crews of the R/V Marion Dufresne, Georges Petit, Korotneff and Catherine Laurence for their assistance in deploying and recovering the sediment trap moorings. The IAEA Marine Environment Laboratory operates under an agreement between the International Atomic Energy Agency and the Government of the Principality of Monaco.

References

[I] FUKAI, R., HOLM, E., BALLESTRA, S., A note on vertical distribution of plutonium and americium in the Mediterranean Sea. Oceanol. Acta 2: 129-132 (1979).

[2] FUKAI, R., BALLESTRA, S., VAS, D., Characteristics of the vertical transport of transuranic elements through the Mediterranean water column, p. 95-101. In VPS Journees d'Etudes sur les Pollutions Marines en Mediterranee. Comm. Internat. Explorat. Scientif. Mer Medit., Monaco (1983).

[3] FOWLER, S.W., BALLESTRA, S., LA ROSA, J., HOLM, E., LOPEZ, J.J., Flux of transuranium nuclides in the northwestern Mediterranean following the Chernobyl accident.

Rapp. Comm. intemat. Mer Medit. 32(1): 317 (1990a).

[4] FOWLER, S.W., BALLESTRA, S., VELLENEUVE, J.-P., Flux of transuranium nuclides and chlorinated hydrocarbons in the northwestern Mediterranean. Continental Shelf Res. 10(9-11):

1005-1023 (1990b).

[5] LIVINGSTON, H.D., ANDERSON, R.F., Large particle transport of plutonium and other fallout radionuclides to the deep ocean. Nature 303: 228-231 (1983).

[6] BALLESTRA, S., FUKAI, R., An improved radiochemical procedure for low-level measurements of americium in environmental matrices. Talanta 30: 45-48 (1983).

[7] MIQUEL, J.-C., FOWLER, S.W., LA ROSA, J., BUAT-MENARD, P., Dynamics of the downward flux of particles and carbon in the open northwestern Mediterranean Sea. Deep-Sea Res. 141(2): 243-261 (1994).

[8] CHRISTENSEN, J.P., PACKARD, T.T., DORTCH, F.Q., MINAS, H.J., GASCARD, J.C., RICHEZ, C, GARFIELD, P.C., Carbon oxidation in the deep Mediterranean sea: evidence for dissolved organic carbon source. Glob. Biogeochem. Cycles 3(4): 315-335 (1989).

[9] HARDY, E.P., KREY, P.W., VOLCHOK, H.L., Global fallout inventory and distribution of fallout plutonium. Nature 241: 444-445 (1973).

[10] RYAN, T.P., MITCHELL, P.I., SANCHEZ-CABEZA, J.A., SMITH, V., VFVES i BATLLE, J., Distribution of radioactive fallout throughout Ireland, p. 276-282. In Proc. Int. Tyndall School and National Environment Week, Carlow (Ireland), 11-19 September 1993. Science, Green Issues and the Environment: Ireland and the Global Crisis, (1995).

[II] LIVINGSTON, H.D., BOWEN, V.T., BURKE, J.C., Fallout radionuclides in Mediterranean sediments, 24: 37-40. Rapports et Proces-Verbaux des Reunions, Comm. Internat. Explorat.

Scientif. Mer Medit., Monaco (1977).

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