Reference Methods for Marine Radioactivity Studies II
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TECHNICAL REPORTS SERIES No. 169 Reference Methods for Marine Radioactivity Studies II INTERNATIONAL ATOMIC ENERGY AGENCY, VIENNA, 1 975 REFERENCE METHODS FOR MARINE RADIOACTIVITY STUDIES II The following States are Members of the International Atomic Energy Agency: AFGHANISTAN HAITI PARAGUAY ALBANIA HOLY SEE PERU ALGERIA HUNGARY PHILIPPINES ARGENTINA ICELAND POLAND AUSTRALIA INDIA PORTUGAL AUSTRIA INDONESIA ROMANIA BANGLADESH IRAN SAUDI ARABIA BELGIUM IRAQ SENEGAL BOLIVIA IRELAND SIERRA LEONE BRAZIL ISRAEL SINGAPORE BULGARIA ITALY SOUTH AFRICA BURMA IVORY COAST SPAIN BYELORUSSIAN SOVIET JAMAICA SRI LANKA SOCIALIST REPUBLIC JAPAN SUDAN CAMBODIA JORDAN SWEDEN CANADA KENYA SWITZERLAND CHILE KOREA, REPUBLIC OF SYRIAN ARAB REPUBLIC COLOMBIA KUWAIT THAILAND COSTA RICA LEBANON TUNISIA CUBA LIBERIA TURKEY CYPRUS LIBYAN ARAB REPUBLIC UGANDA CZECHOSLOVAKIA LIECHTENSTEIN UKRAINIAN SOVIET SOCIALIST DEMOCRATIC PEOPLE'S LUXEMBOURG REPUBLIC REPUBLIC OF KOREA MADAGASCAR UNION OF SOVIET SOCIALIST DENMARK MALAYSIA REPUBLICS DOMINICAN REPUBLIC MALI UNITED KINGDOM OF GREAT ECUADOR MAURITIUS BRITAIN AND NORTHERN EGYPT MEXICO IRELAND EL SALVADOR MONACO UNITED REPUBLIC OF ETHIOPIA MONGOLIA CAMEROON FINLAND MOROCCO UNITED STATES OF AMERICA FRANCE NETHERLANDS URUGUAY GABON NEW ZEALAND VENEZUELA GERMAN DEMOCRATIC REPUBLIC NIGER VIET-NAM GERMANY, FEDERAL REPUBLIC OF NIGERIA YUGOSLAVIA GHANA NORWAY ZAIRE GREECE PAKISTAN ZAMBIA GUATEMALA PANAMA The Agency's Statute was approved on 23 October 1956 by the Conference on the Statute of the IAEA held at United Nations Headquarters, New York; it entered into force on 29 July 1957. The Headquarters of the Agency are situated in Vienna. Its principal objective is "to accelerate and enlarge the contribution of atomic energy to peace, health and prosperity throughout the world". Printed by the IAEA in Austria July 1975 TECHNICAL REPORTS SERIES No. 169 REFERENCE METHODS FOR MARINE RADIOACTIVITY STUDIES II Sampling techniques and analytical procedures for the determination of selected radionuclides and their stable counterparts II: Iodine, ruthenium, silver, zirconium and the transuranic elements INTERNATIONAL ATOMIC ENERGY AGENCY VIENNA, 1975 The International Laboratory of Marine Radioactivity operates under a tripartite agreement between the International Atomic Energy Agency, the Government of Monaco and the Oceanographic Institute. REFERENCE METHODS FOR MARINE RADIOACTIVITY STUDIES II IAEA, VIENNA, 1975 STI/DOC/10 /169 ISBN 92-0-125275-7 FOREWORD The present technical report complements that published as Technical Reports Series No. 1 18 by the International Atomic Energy Agency in 1970. Since, at that time, information on certain radionuclides of importance in the context of waste releases into the marine environment was not covered by the report, the necessity of further studies was emphasized. A second panel on the Reference Methods for Marine Radioactivity Studies was convened by the International Atomic Energy Agency from 30 October to 3 November 1972 in Vienna to study the available information on current analytical methods for transuranic elements and radioruthenium, and for the radionuclides of zirconium, silver and iodine. It was intended to assist researchers by presenting critical reviews of possible reference methods for analysis of these radionuclides. The global energy situation calls for a faster rate of expansion of the nuclear industry. It is therefore imperative that the impact of such an expansion on the environment should be carefully evaluated on a sound scientific basis. It is hoped that this report will contribute to the production of reliable data in radionuclide measurements on the marine environmental samples, thus in turn contributing to safeguarding the quality of human life. CONTENTS I. INTRODUCTION 1 1. General scope and main objectives 1 2. Working procedures 2 3. Members of the Study Group • • • 2 II. TRANSURANIC ELEMENTS 5 1. Introduction 5 2. Sample collection 6 3. Sample storage 11 4. Sample processing 13 5. Radioanalytical procedures 17 6. Presentation of data 29 Ul. RADIORUTHENIUM 33 1. Introduction 33 2. Chemical behaviour in the marine environment 34 3. Determination in seawater samples 36 4. Determination on biological materials and sediments 39 5. General remarks 41 IV. Z1RCONIUM-95 (N10B1UM-95) 43 1. Introduction 43 2. Sample collection and storage 43 3. Pretreatment and concentration 44 4. Methods for determination 44 5. Data interpretation 46 6. General remarks , 46 V. RADIOACTIVE AND STABLE SILVER 47 1. Introduction 47 2. Sampling, storage and pretreatment 47 3. Determination of radiosilver 48 4. Determination of stable silver 49 5. General remarks 49 VI. RADIOIODINE 51 1. lodine-131 51 2. Other radioisotopes of iodine 53 3. General remarks 54 VII. GENERAL RECOMMENDATIONS 55 REFERENCES 57 SUPPORTING PAPERS Quality control in radiochemical analysis 63 J.H. Harley, H.L. Volchok, V.T. Bowert Double-tracer studies to optimize conditions for the radiochemical separation of plutonium from large seawater samples 69 H. D. Livingston, D. R. Mann, V. T. Bowen A procedure for analysis of americium in marine environmental samples 77 R. Bojanowski, ¡i.D. Livingston, D.L. Scheider, D.R. Mann Isotopic analysis of plutonium in environmental samples by isotopic dilution mass spectrometry 87 R.J. Dupzyk, R.D. Carver, I.A. Dupzyk Procedure for plutonium analysis of large (100 g) soil and sediment samples 89 J. W. T. Meadows, J.S. Schweiger, B. Mendoza, R. Stone Radiochemical determination of plutonium in marine samples by ion exchange and solvent extraction 91 A. Aarkrog Determination of plutonium in the marine environment 97 K.C. Pillai Results of plutonium intercalibration in seawater and seaweed samples 107 R. Fukai, C.N. Murray Methods of ruthenium-106 analysis in marine environmental samples: A review 121 M. Shiozaki, N. Yamagata, K. Iwashima Determination of radionuclides of Ce, Co, Fe, Ru, Zn and Zr in seawater by prcconcentration of colloidal manganese dioxide: Application to the determination of low-level ruthenium-106 137 P. Guéguéniat, R. Camion, Y. Lucas Radioruthenium in coastal waters 147 K.C. Pillai, NN. Dey A review of methods for the determination of radioactive and stable zirconium in the marine environment 155 J. W. R. Dutton A review of methods for the determination of radioactive and stable silver in the marine environment 163 J. W.R. Dutton A review of methods for the determination of iodine-131 in the marine environment 173 J. W.R. Dutton A rapid method for the determination of radioiodine in suspended matter and seawater 177 5. Wlodek A method for the rapid enrichment and determination of silver-1 10m and iodine-131 from seawater 179 H.-F Eicke A study of the stability of some radionuclides in seawater 187 J.W.R. Dutton, R.D. lbbett, I.E. Woolner Intercalibration of methods for radionuclide measurements on a seaweed sample 213 R. Fukai, S. Ballestra Radioactivity in the hydrosphere: Recent trends in Czech studies 235 A. Mansfeld I. INTRODUCTION 1. GENERAL SCOPE AND MAIN OBJECTIVES Under its Statute the International Atomic Energy Agency is entrusted with promulgating standards and in drawing up internationally acceptable regulations to prevent pollution of the sea by radioactive materials in amounts that would adversely affect man and his marine resources [ 1] . To implement these tasks the Agency has convened several panels of leading experts on the relevant subjects. The reports of these panels have already been published [2-4], One of the important aspects of environmental protection against radio- active contamination is the monitoring of radionuclides released into the environment by nuclear operations. Since the monitoring data constitute the basis for preventive measures or regulatory actions against pollution, the quality of the data should be sufficiently accurate to permit the linking of the data with the radiation doses received by man and his environment. On the other hand, extensive studies are still required to understand the behaviour of radionuclides in the marine environment. These studies are imperative for obtaining the basis of predictions of the fate of radionuclides released, as well as for understanding the biogeochemical processes prevailing in the marine environment. Since the sea is considered as both an immediate and an ultimate sink of the radionuclides released into the environment and, at the same time, interconnects national territories, the results of radio- nuclide measurements, particularly on marine environmental samples, are required to be comparable on an international basis. Up to the present this requirement was not always fulfilled. To find a solution for the required improvement of the comparability of measurements, an ad hoc panel was convened in November 1968 to study the possibility of presenting sets of reference analytical methods for radionuclides of strontium, caesium, cerium, cobalt and zinc, together with their corresponding stable counter- parts, including the collection, storage and preparation of samples for chemical and radiochemical analyses. The report of this panel was published in the Technical Report Series [ 5] . Since the above-mentioned radionuclides were selected not on the basis of their importance as marine radioactive contaminants, but because relatively abundant data existed on them in a marine context, the panel pointed out at that time that further studies would be necessary on other radionuclides of importance when sufficient data became available. The panel also recommended that the