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Control of Semivolatile Radionuclides in Gaseous Effluents at Nuclear Facilities

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Control of Semivolatile Radionuclides in Gaseous Effluents at Nuclear Facilities TECHNICAL REPORTS SERIES No. Control of Semivolatile Radionuclides in Gaseous Effluents at Nuclear Facilities INTERNATIONAL ATOMIC ENERGY AGENCY, VIENNA, 1982 CONTROL OF SEMIVOLATILE RADIONUCLIDES IN GASEOUS EFFLUENTS AT NUCLEAR FACILITIES The following States are Members of the International Atomic Energy Agency: AFGHANISTAN HOLY SEE PHILIPPINES ALBANIA HUNGARY POLAND ALGERIA ICELAND PORTUGAL ARGENTINA INDIA QATAR AUSTRALIA INDONESIA ROMANIA AUSTRIA IRAN ISLAMIC REPUBLIC SAUDI ARABIA BANGLADESH IRAQ SENEGAL BELGIUM IRELAND SIERRA LEONE BOLIVIA ISRAEL SINGAPORE BRAZIL ITALY SOUTH AFRICA BULGARIA IVORY COAST SPAIN BURMA JAMAICA SRI LANKA BYELORUSSIAN SOVIET JAPAN SUDAN SOCIALIST REPUBLIC 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 JAMAHIRIYA UGANDA CZECHOSLOVAKIA LIECHTENSTEIN UKRAINIAN SOVIET SOCIALIST DEMOCRATIC KAMPUCHEA LUXEMBOURG REPUBLIC DEMOCRATIC PEOPLE'S MADAGASCAR UNION OF SOVIET SOCIALIST REPUBLIC OF KOREA MALAYSIA REPUBLICS DENMARK MALI UNITED ARAB EMIRATES DOMINICAN REPUBLIC MAURITIUS UNITED KINGDOM OF GREAT ECUADOR MEXICO BRITAIN AND NORTHERN EGYPT MONACO IRELAND EL SALVADOR MONGOLIA UNITED REPUBLIC OF ETHIOPIA MOROCCO CAMEROON FINLAND NETHERLANDS UNITED REPUBLIC OF FRANCE NEW ZEALAND TANZANIA GABON NICARAGUA UNITED STATES OF AMERICA GERMAN DEMOCRATIC REPUBLIC NIGER URUGUAY GERMANY, FEDERAL REPUBLIC OF NIGERIA VENEZUELA GHANA NORWAY VIET NAM GREECE PAKISTAN YUGOSLAVIA GUATEMALA PANAMA ZAIRE HAITI PARAGUAY ZAMBIA PERU 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". © IAEA, 1982 Permission to reproduce or translate the information contained in this publication may be obtained by writing to the International Atomic Energy Agency, Wagramerstrasse 5, P.O. Box 100, A-1400 Vienna, Austria. Printed by the IAEA in Austria December 1982 TECHNICAL REPORTS SERIES No. 220 CONTROL OF SEMIVOLATILE RADIONUCLIDES IN GASEOUS EFFLUENTS AT NUCLEAR FACILITIES INTERNATIONAL ATOMIC ENERGY AGENCY VIENNA, 1982 CONTROL OF SEMIVOLATILE RADIONUCLIDES IN GASEOUS EFFLUENTS AT NUCLEAR FACILITIES IAEA, VIENNA, 1982 STI/DOC/10/220 ISBN 92-0-125482-2 FOREWORD In the context of an expanding nuclear fuel cycle, where more and more electrical power is generated by nuclear fission, increased attention is being paid to control of releases of radioactive effluents to the environment. To assist £ national authorities responsible for restricting the discharge of effluents in order to limit population exposure, the International Atomic Energy Agency has undertaken a programme to collect, review and disseminate information on technologies for handling and treatment of gaseous and particulate radioactive wastes from nuclear facilities. The IAEA's programme of work covers different aspects of radioactive airborne effluents and wastes. The results of IAEA meetings on handling krypton-85, radioiodine and tritium have been published in the Agency's Technical Reports Series, as follows: Separation, Storage and Disposal of Krypton-85, Technical Reports Series No. 199, IAEA, Vienna (1980). Radioiodine Removal in Nuclear Facilities: Methods and Techniques for Normal and Emergency Situations, Technical Reports Series No. 201, IAEA, Vienna (1980). Further documents are in preparation on the retention of gaseous radionuclides from nuclear power plants under normal and accident conditions and on testing and in-plant monitoring of offgas cleaning systems. A Symposium on Management of Gaseous Wastes from Nuclear Facilities, jointly organized by IAEA and OECD-NEA in Vienna in 1980, and published by the IAEA in 1980, dealt with current practice and the latest developments in the field. The contents of this Technical Report are based on the results of a Techni- cal Committee Meeting on Retention of Semivolatile Radionuclides at Nuclear Facilities, held in Vienna from 27 to 31 October 1980. Additional information was collected subsequently from the USA, the USSR and India and has been incorporated. The information contained in this report represents an up-to-date review of the subject, combining the results of laboratory studies on control of the most important semivolatile radionuclides in gaseous effluents at nuclear facilities and the results of operating experience in that area. The Agency wishes to express its thanks to all participants of the meeting, particularly to M. Klein, Belgium, who served as Chairman. The Agency is also grateful to those who contributed information after the meeting, particularly to H. Deuber, Federal Republic of Germany, who as a consultant to the Agency collected most of this information and compiled the present report. The officer of the IAEA responsible for this work was V. Tsyplenkov of the Waste Manage- ment Section. CONTENTS 1. INTRODUCTION 1 2. SIGNIFICANCE OF THE CONTROL OF SEMIVOLATILES 1 2.1. Solidification of high-level liquid waste (HLLW) 3 2.2. Reprocessing of nuclear fuel 3 3. PROPERTIES OF RUTHENIUM 5 3.1. Volatilization of ruthenium 5 3.1.1. Volatilization of ruthenium at low temperatures 5 3.1.2. Volatilization of ruthenium at high temperatures 8 3.2. Deposition of ruthenium 10 3.3. Retention of ruthenium 14 3.3.1. Retention of ruthenium by solids 14 — General - Silica gel — Ferric-oxide-based materials - Catalytic decomposition 3.3.2. Retention of ruthenium by liquids 18 4. PROPERTIES OF OTHER SEMIVOLATILES 18 4.1. Properties of caesium 19 4.2. Properties of selenium, technetium, antimony and tellurium 19 5. PRINCIPLES OF HIGH-LEVEL WASTE SOLIDIFICATION PROCESSES 20 5.1. Solidification methods 20 5.2. Offgas treatment systems 21 5.2.1. Individual components 23 5.2.2. Integrated systems 23 6. EXPERIENCE WITH CONTROL OF SEMIVOLATILES IN HIGH-LEVEL LIQUID WASTE SOLIDIFICATION PROCESSES 24 6.1. Fluidized-bed calcination 24 6.2. Spray calcination 30 6.3. Rotary-kiln calcination 33 6.4. Pot calcination 35 6.5. Liquid-fed ceramic melter 46 6.6. Summary 48 7. SAMPLING AND MONITORING 49 8. CONCLUSIONS 50 REFERENCES 51 LIST OF PARTICIPANTS 55 1. INTRODUCTION The contaminants in gaseous effluents of nuclear facilities are usually con- sidered to consist of particulates and gases. There are, however, also contaminants which are generally present in the condensed form and which volatilize significantly owing to rise in temperature or chemical reactions. These semivolatile contaminants may not be trapped sufficiently by the devices commonly used for decontaminating the gaseous effluents of nuclear facilities and may therefore have to be dealt with separately. The semivolatile contaminants include isotopes of selenium, technetium, ruthenium, antimony, tellurium and caesium. This report reviews the present knowledge of control of these semivolatiles in the gaseous effluents of nuclear facilities under normal conditions. The main topics of this report have been reviewed up to 1976, and up to 1977 in Refs [1—3]. The literature contained in these reviews is taken into account in this report, although it is not usually cited unless tables or figures are reproduced. The emphasis is, rather, on quoting literature published later. 2. SIGNIFICANCE OF THE CONTROL OF SEMIVOLATILES The significance of control of radionuclides in gaseous effluents may be related both to the environmental impact and to the influence within the facilities. The environmental impact may be characterized by the efforts necessary to comply with the retention requirements which are determined by the activity inventories or processing rates and the maximum permissible releases of the radionuclides. Thus, apart from the retention requirement, the environmental impact depends on the release potential and the behaviour of the radionuclides in the offgas treatment system. The significance in terms of the impact within the plants is associated with the creation of high radiation fields in unshielded areas, plugging of pipes due to deposition, and contamination of secondary-effluent streams. Apart from activity, mass is an important factor in this context. As will be shown later, semivolatiles may volatilize to a large extent with high temperatures and/or oxidizing conditions. Therefore, in normal operation it is only in solidification of high-level liquid waste (HLLW) and in reprocessing nuclear fuel that appreciable volatilization of semivolatiles has to be reckoned with. Only these processes will be considered further. 1 TABLE I. CONTENT OF RADIONUCLIDES IN LWR HIGH-LEVEL LIQUID WASTE3 [2] Isotope Half-life Activity Mass 1 (Ci-r1 U) (g-r u) Volatile H-3 12.33 a 33 3.5 X 10"J Kr-85 10.73 a 8X10"3 2.0 X 10"s 1-129 1.59 X 107 a 3 X 10"s 0.2 Potentially volatile Se-79. 6.5 X 104 a 0.34 4.9 Tc-99 2.13 X 105 a 13 7.4 X 102 Ru-103 0.1084 a 72 2.2 X 10~3 Ru-106 1.01 a 1.8 X 10s 54 b Rh-103m 56 min 72 - b s Rh-106 29.9 s 1.8 X 10 - Te-123m 0.3275 a 1.5 X 10"2 1.8 X 10"6 Te-127m 0.298 a 4.2 X 102 4.5 X 10~2 Sb-124 0.1648 a 0.68 3.9 X 10"5 Sb-125 2.73 a 5.7 X 103 5.5 Sb-126mb 19.0 min 0.54 . 6.8 X 10"' Sb-126b 12.4 d 0.53 6.4 X 10"6 Cs-134 . 2.06 a 1.2 X 10s 91 Cs-135 2.3 X 106 a 0.31 2.7 X 102 Cs-137 30.1 a 9.3 X 104 1.1 X 103 Potential solids (major activities only)0 s Ce-144 0.7787 a 2.4 X 10 - b s Pr-144 17.28 min 2.4 X 10 - 4 Sr-90 29 a 6.0 X 10 - b 4 Y-90 64.0 h 6.0 X 10 - 3 Cm-244 • 17.9a 7.0 X 10 _ Note: 1 curie (Ci)= 3.70 X 1010 Bq.
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