TECHNETIUM IN THE ENVIRONMENT

Proceedings of a Seminar on the Behaviour of Technetium in the Environment, organised by the Commission of the European Communi­ties, Radiation Protection Programme, and the Service d'Etudes et de Recherches sur l'Environnement of the Commissariat it l'Energie Atomique, France, in collaboration with the Office of Health and Environmental Research of the Department of Energy, USA, and held

at Cadarache (France), 23-26 October 1984.

PROGRAMME COMMITTEE

A. Grauby, France H. Smith, UK R. Kirchmann, Belgium P. Scoppa, Commission of the European Communities C. Myttenaere, Commission of the European Communities A. Cigna, Italy E. Holm, Sweden O. Hoffman, USA

TECHNETIUM IN THE ENVIRONMENT

Edited by

G. DESMET and C. MYTTENAERE Commission of the European Communities.

Radiation Protection Programme

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© ECSC, EEC, EAEC, BRUSSELS AND LUXEMBOURG, 1986 Softcover reprint of the hardcover 1st edition 1986

British Library Cataloguing in Publication Data

Technetium in the environment. I. Technetium-Environmental aspects I. Desmet, G. II. Myttenaere, C. 363.7'384 TD196.T4

Library of Congress Cataloging-in-Publication Data

Seminar on the Behaviour of Technetium in the Environment (1984: Cadarache, France) Technetium in the environment.

"Proceedings of a Seminar on the Behaviour of Technetium in the Environment, organised by the Commission of the European Communities, Radiation Protection Programme, and the Service d'etudes et de recherches sur l'environnement of the Commissariat a I'energie atomique, France, in collaboration with the Office of Health and Environmental Research of the Department of Energy, USA, and held at Cadarache (France), 23-26 October 1984"-P. ii.

Bibliography: p. Includes index. I. Technetium-Environmental aspects--Congresses.

I. Desmet, G. II. Myttenaere, C. III. Commission of the European Communities. Radiation Protection Programme. IV. France. Service d'etudes et de recherches sur I'environnement. V. United States. Dept. of Energy. Office of Health and Environmental Research. VI. Title. QH545.T37S46 1984 574.5'222 85-29221

ISBN -13:978-94-010-8361-4 e-ISBN-13 :978-94-009-4189-2 DOl: 10.1007/978-94-009-4189-2

Publication arrangements by: Commission of the European Communities, Directorate­General for the Information Market and Innovation, Luxembourg

EUR 10102 EN

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PREFACE

Since the discovery of technetium (in 1937, by Perrier and Segre), technetium-99 and technetium-99m have become most familiar in the specialised literature, the behaviour of the former being of concern regarding its health impact, the latter having been used intensively in medical tests for many years. The knowledge of the characteristics and behaviour of this element in nature is currently increasing exponentially. It has become clear, however, that there is still a serious shortage of information needed to assess properly its burden and impact on man and his environment.

Technetium may indeed be released from nuclear installations or as a waste product from medical applications. It is generally considered to be highly mobile as the anion TcOi, but it is also suspected to be readily reduced in soils and metabolised in living beings into lower oxidation states.

The seminar was planned to analyse thoroughly the experimental results obtained up to now and to make recommendations of specific issues requiring further research. This book presents the papers of the different sessions in the order of presentation, and the conclusions drawn by three discussion groups which dealt separately with:

problems of sources and distribution of man-made technetium and its radiological consequences; the chemical behaviour of technetium in different ecosystems; biochemical reactions and binding with macromolecules in various life systems.

vi Preface

The editors, together with the Programme Committee of the Seminar, wish to express their gratitude to the chairmen of the different sessions for their summary of the group discussions.

The publication of these proceedings enables the organisers of this seminar to draw attention to this specific element in the table of Mendeleev, with its multifarious and intensive utilisation in medical research, but with its paradoxically relatively unknown basic behaviour in the environment.

THE EDITORS

CONTENTS

Preface .

1. Source Terms for Technetium-99 from Nuclear Fuel Cycle Facilities .

J. E. TILL (Radiological Assessments Corporation, Neeses, South Carolina, USA)

v

2. Technetium Discharges into the Environment 21 F. LUYKX (Commission of the European Communities, Lux­embourg)

3. Radiochemical Determination of Tc-99 and Release of Tc-99 from Nuclear Facilities . 29

B. BOHN, H. J. LUXENBURGER and H. SCHUTTELKOPF (KernJorschungszentrum Karlsruhe GmbH, Karlsruhe, Fed-eral Republic of Germany)

4. Activites du Technetium 99 Mesurees dans les Eaux Residu­aires, l'Eau de Mer et Deux Bioindicateurs (Littoral de la Manche, 1983) . 37

F. PATTI (Service d'Etudes App/iquees de Protection San-itaire, Fontenay aux Roses, France), M. MASSON (Service d'Etudes et de Recherches sur L'Environnement, Cherbourg, France), G. VERGNAUD (Service de Prevention et de Radio­protection, Cherbourg, France) and L. JEANMAIRE (Service d'Etudes Appliquees de Protection Sanitaire, Fontenay aux Roses, France)

VlI

viii Contents

5. Technetium-99 in Algae from Temperate and Arctic Waters of the North Atlantic. 53

E. HOLM (International Laboratory of Marine Radioactivity, Monaco), J. RIOSECO (Department of Radiation Physics, Lund University, Sweden), A. AARKROG, H. DAHLGAARD (Riso National Laboratory, Roskilde, Denmark), L. HALLsTADIus, B. BJURMAN and R. HEDvALL (Department of Radiation Physics, Lund University, Sweden) G. M. DESMET (Commission of the European Communities, Brussels, Belgium)

6. Technetium-99 in the Baltic Sea E. HOLM (International Laboratory of Marine Radioactivity, Monaco), J. RIOSECO (Department of Radiation Physics, Lund University, Sweden) and S. MATTSSON (Department of Radiation Physics, University of Gothenburg, Sweden)

61

7. Time Trend of 99Tc in Seaweed from Greenland Waters 69 A. AARKROG, H. DAHLGAARD (Riso National Laboratory, Roskilde, Denmark), L. HALLSTADIUS (Department of Radi-ation Physics, Lund University, Sweden), E. HOLM (Inter­national Laboratory of Marine Radioactivity, Monaco), S. MATTSON (Department of Radiation Physics, University of Gothenburg, Sweden) and J. RIOSECO (Department of Radiation Physics, Lund University, Sweden)

8. Behaviour of Technetium in Freshwater Environments 79 B. G. BLAYLOCK, M. L. FRANK, F. O. HOFFMAN and D. L. DEANGELIS (Oak Ridge National Laboratory, Tennessee, USA)

9. Role of Organic Matter as a Geochemical Sink for Technetium in Soils and Sediments 91

M. STALMANS, A. MAES and A. CREMERS (Fakulteit der Landbouwwetenschappen, KU Leuven, Belgium)

10. Technetium Sorption in Surface Soils 115 R. E. WILDUNG, T. R. GARLAND, K. M. McFADDEN and C. E. COWAN (Pacific Northwest Laboratory, Richland, Washington, USA)

Contents ix

11. Technetium Behaviour in Soils of the Canadian Precambrian Shield . 131

M.1. SHEPPARD and S. C. SHEPPARD (Atomic Energy Canada Limited, Pinawa, Manitoba, Canada)

12. Soil-Humic Acid Complexes of Technetium: Synthesis and Characterisation 143

L. VAN LOON, M. STALMANS, A. MAES, A. CREMERS and M. COGNEAU (Fakulteit der Landbouwwetenschappen, KU Leuven, Belgium)

13. Measurement of the Complexation Capacity of Organic Matter in Dilute Extracts of Soils and Sediments . 155

M. STALMANS, S. DE KEIJZER, A. MAES and A. CREMERS (Fakulteit der Landbouwwetenschappen, KU Leuven, Belgi-um)

14. 99Tc in Environmental Waters 169 M. GARciA-LEON, C. PIAZZA and G. MADURGA (Universidad de Sevilla, Spain)

15. Properties and Solubility of Technetium Dioxide 179 CH. HANKE, B. JAHRLlNG and K. H. LIESER (Technische Hochschule Darmstadt, Federal Republic of Germany)

16. Relevance of the Study of Technetium Accumulation and Speciation in Plants 189

17. A Review of the Biological and Geochemical Behaviour of Technetium in the Marine Environment 197

T. M. BEASLEY and H. V. LORZ (College of Oceanography, Oregon State University, Corvallis, USA)

18. Accumulation and Loss of Technetium by Macrophytic Algae 217 C. BENco, S. CANNARSA, I. CEPPODOMO and A. ZATTERA (ENEA Centro Ricerche Energia Ambiente, La Spezia, Italy)

x Contents

19. Technetium in Micro-organisms 229 B. MANIA, Z. MOUREAU, D. VAN DER BEN (lnstitut Royal des Sciences Naturelles de Belgique, Brussels, Belgium), J. VAN BAELEN (CEN-SCK, Mol, Belgium), C. VERTHE, J. M. BOUQUEGNEAU (lnstitut de Chimie, Universite de Liege, Belgium), M. COONEAU (Laboratoire de Chimie Nuc/eaire, Universite Catholique de Louvain, Belgium), S. BONOTTO (CEN-SCK, Mol, Belgium), C. M. VANDECASTEELE, L. PIGNOLET (Laboratoire de Physiologie Vegetale, Universite Catholique de Louvain, Belgium) and C. MYTTENAERE (Com­mission of the European Communities, Brussels, Belgium)

20. Technetium in Marine Animals 245 C. VERTHE (lnstitut de Chimie, Universite de Liege, Belgium), Z. MOUREAU, B. MANIA (lnstitut Royal des Sciences Natur-elles de Belgique, Brussels, Belgium), J. VAN BAELEN (CEN-SCK, Mol, Belgium), D. VAN DER BEN (lnstitut Royal des Sciences Naturelles de Belgique, Brussels, Belgium), M. COGNEAU (Laboratoire de Chimie Nuc/eaire, Universite Catholique de Louvain, Belgium), C. M. VANDECASTEELE (Laboratoire de Physiologie Vegetale, Universite Catholique de Louvain, Belgium), J. M. BOUQUEGNEAU (lnstitut de Chimie, Universite de Liege, Belgium), C. MYTTENAERE (Commission of the European Communities, Brussels, Belgium) and S. BONOTTO (CEN-SCK, Mol, Belgium)

21. LeTechnetium et l'Ormeau (Haliotis tuberculata): Donnees Experimentales et 'in situ' 251

M. MASSON (lPSN-DERS-SERE, Cherbourg, France), G. APROSI (Electricite de France, Chatou, France) and P. GERMAIN (lPSN-DERS-SERE, Cherbourg, France)

22. Plant Root Absorption and Metabolic Fate of Technetium in Plants 265

D. A. CATALDO, T. R. GARLAND and R. E. WILDUNG (Pacific Northwest Laboratory, Richland, Washington, USA)

Contents xi

23. Processus Biologiques Responsables de l'Accumulation du Tc-99 par les Vegetaux 281

c. MYTTENAERE (Commission of the European Communities, Brussels, Belgium), C. M. VANDECASTEELE, P. Roucoux, E. A. LIETART, A. ITSCHERT (Laboratoire de Physiologie Vegetale, Universite Catholique de Louvain, Belgium) and 1. MOUSNY (Commission of the European Communities, Brussels, Belgium)

24. Accumulation of Tc-Bio-organic Complexes in Spinach Plants in Relation to Growth 295

1. F. M. M. LEMBRECHTS and G. M. DESMET (NIPHEH, Laboratory of Radiation Research, Wageningen, The Nether-lands)

25. Speciation of Technetium in Plants Grown on Substrates which Contained Different Chemical Forms of Technetium 301

L. R. VAN LooN and 1. F. M. M. LEMBRECHTS (NIPHEH, Laboratory of Radiation Research, Wageningen, The Nether-lands)

26. Retention par les Vegetaux du Technetium Relache dans l'Environnement en Association avec d'Autres Radiopolluants 307

P. Roucoux and C. COLLE (CEA-IPSN, Saint Paul-Iez­Durance, France)

27. Chemical Form of Technetium in Corn (Zea mays) and the Gastrointestinal Absorption of Plant-incorporated Tc by Laboratory Rats 319

C. T. GARTEN, JR (Oak Ridge National Laboratory, Tennes-see, USA), C. MYTTENAERE, C. M. VANDECASTEELE (Labor-atoire de Physiologie Vegetale, Universite Catholique de Louvain, Belgium), R. KIRCHMANN and R. VAN BRuWAENE (CEN-SCK, Mol, Belgium)

xii Contents

28. Absorption and Retention in Sheep of Technetium Adminis-tered into the Rumen as Pertechnetate or Bound to Food 333

R. VAN BRUWAENE, G. B. GERBER, R. KIRCHMANN (Centre d'Etude de I'Energie Nuc/eaire, Mol, Belgium), C. T. GARTEN, JR. (Oak Ridge National Laboratory, Tennessee, USA), J. V ANKERKOM, S. BONOTTO, T. MATHIEU (Centre d'Etude de I'Energie Nuc/eaire, Mol, Belgium) and M. COGNEAU (Laboratoire de Chimie Inorganique et Nuc/eaire, Universite Catholique de Louvain, Belgium)

29. Transfer of 1311 and 95mTc from Pasture to Goat Milk 339 E. A. BONDlETT! and C. T. GARTEN, JR (Oak Ridge National Laboratory, Tennessee, USA)

30. Distribution of Orally Administered and ChronicaIIy Fed 95mTc in Japanese Quail Tissues and Eggs 349

J. M. THOMAS, L. L. CADWELL, D. A. CATALDO and T. R. GARLAND (Pacific Northwest Laboratory, Richland, Wash-ington, USA)

31. The Significance of Environmental Exposure Pathways for Technetium 359

F. O. HOFFMAN, R. H. GARDNER and S. M. BARTELL (Oak Ridge National Laboratory, Tennessee, USA)

32. Estimations des Risques Radiologiques Lies a un Rejet Con-certe de Technetium dans I'Environnement 377

J. QUINAULT and A. GRAUBY (CEN Cadarache, Saint Paul-lez-Durance, France)

33. Interaction entre Technetium et Molybdene dans l'Inhibition de la Nitrogenase d'Azotobacter Chroococcum 385

C. M. VANDECASTEELE, J. HENROT (Laboratoire de Physio-logie Vegetale, Universite Catholique de Louvain, Belgium), J. M. PIERI (Laboratoire de Biochimie, Universite de Nantes, France), C. MYTTENAERE (Commission of the Euro-pean Communities, Brussels, Belgium), M. COGNEAU (Labora-toire de Chimie Nuc/eaire, Universite Catholique de Louvain, Belgium) and C. V AN HOVE (Laboratoire de Physiologie Vegetale, Universite Catholique de Louvain, Belgium)

Contents xiii

34. Toxicity of Long-tenn Application of Dietary Technetium to Rats and their Offspring. 391

R. VAN BRUWAENE, M. HEGELA, G. B. GERBER, R. KIRCHMANN and J. R. MAISIN (Centre d'Etude de I'Energie Nuc/eaire, Mol, Belgium)

Summary of the Oral Presentations

Summaries of the Discussions of the Working Groups

List of Participants

Index

397

399

403

405