U Uranium: Behavior of Uranium Fuels in Nuclear Reactors. Reprocessing of Spent Nuclear Fuels PDF
Preview U Uranium: Behavior of Uranium Fuels in Nuclear Reactors. Reprocessing of Spent Nuclear Fuels
Gmelin Handbook of lnorganic Chemistry 8th Edition Gmelin Handbock Volumes on Radium and Actinides Ac Actinium* - 1942 Actinium Suppl. Vol. 1 - 1981 Np,Pu ... PartA1, I (New Suppl. Series Vol. Nr. 7 a) } - 1973 Part A 1, II" (New Suppl. Series Vol. Nr. 7 b) (Elements) - 1974 Part A2o (New Suppl. Series Vol. Nr. 8) - 1973 Part B 1 o (New Suppl. Series Vol. Nr. 31) (Metals) - 1976 Part B2* (New Suppl. Series Vol. Nr. 38) - 1976 } (AIIoys) Part B3* (New Suppl. Series Vol. Nr. 39) - 1977 Part Co (New Suppl. Series Vol. Nr. 4) (Compounds) - 1972 Part D 1 o (New Suppl. Series Vol. Nr. 20) - 1975 } (Chemistry in Solution) Part D2o (New Suppl. Series Vol. Nr. 21) - 1975 Index- 1979 Pa Protactinium Main Volume* - 1942 Protactinium Suppl. Vol. 1 o (Element) - 1977 Protactinium Suppl. Vol. 2° (Metal. Alloys. Compounds. Chemistry in Solution) - 1977 Ra Radium Main Volume* - 1928 Radium Suppl. Vol. 1 * (History. Cosmochemistry. Geochemistry) - 1977 Radium Suppl. Vol. 2 (Element. Compounds) - 1977 Th Thorium Main Volume* - 1955 Thorium Suppl. Vol. C1 * (Compounds with Rare Gases, Hydrogen, Oxygen) - 1978 Thorium Suppl. Vol. C2 * (Ternary and Polynary Oxides) - 1976 u Uranium Main Valurne * - 1936 Uranium Suppl. Vol. A 1 * (Uranium Deposits) - 1979 Uranium Suppl. Vol. A2o (Isotopes) - 1980 Uranium Suppl. Vol. A3 * (Technology. Uses) - 1981 Uranium Suppl. Vol. A4 (lrradiated Fuel. Reprocessing) -1982(present volume) Uranium Suppl. Vol. C1 * (Compounds with Rare Gases and Hydrogen. Uranium-Oxygen System) - 1977 Uranium Suppl. Vol. C2 * (U 0 and U0 Oxides. Hydroxides and Oxide 3 8 3 Hydrates. Peroxides) - 1978 Uranium Suppl. Vol. C3 * (Ternary and Polynary Oxides) - 1975 er Uranium Suppl. Vol. (Compounds with Nitrogen) - 1981 Uranium Suppl. Vol. C8* (Compounds with Fluorine) - 1980 Uranium Suppl. Vol. C9 (Compounds with Chlorine, Bromine,lodine) -1979 Uranium Suppl. Vol. C11 (Compounds with Selenium, Tellurium, and Baron)- 1981 Uranium Suppl. Vol. C14 (Compounds with P, As, Sb, Bi, Ge) - 1981 Uranium Suppl. Vol. D2 (Solvent Extraction) - 1982 Uranium Suppl. Vol. E1 (Coordination Compounds) - 1979 Uranium Suppl. Vol. E2o (Coordination Compounds) - 1980 Completely or o in part in German Grnelin Handbuch der Anorganischen Chemie Achte völlig neu bearbeitete Auflage BEGRÜNDET VON Leopold Gmelin ACHTE AUFLAGE BEGONNEN im Auftrag der Deutschen Chemischen Gesellschaft von R. J. Meyer FORTGEFÜHRT VON E. H. E. Pietsch und A. Kotowski Margot Becke-Goehring HERAUSGEGEBEN VOM Gmelin-lnstitut für Anorganische Chemie der Max-Pianck-Gesellschaft zur Förderung der Wissen schaften Direktor: Ekkehard Fluck Springer-Verlag Berlin Heidelberg GmbH 1982 Gmelin-lnstitut für Anorganische Chemie der Max-Pianck-Gesellschaft zur Förderung der Wissenschaften KURATORIUM (ADVISORY BOARD) Dr. J. Schaafhausen, Vorsitzender (Hoechst AG, Frankfurt/Main-Höchst), Dr. G. Breil (RuhrchemieAG, Oberhausen-Holten), Dr. G. Broja (Bayer AG, Leverkusen), Prof. Dr. G. Fritz (Universität Karlsruhe), Prof. Dr. N. N. Greenwood (University of Leeds), Prof. Dr. R. Hoppe (Universität Gießen), Prof. Dr. R. Lüst ( Präsidentder Max-Pianck-Gesellschaft, München), Dr. H. Moell (BASF-Aktiengesellschaft, Ludwigshafen), Prof. Dr. E. L. Muetterties (University of California,Berkeley,California), Prof. Dr. H. Nöth (Universität München), Prof. Dr.A. Rabenau (Max-Pianck-lnstitut für Festkörperforschung, Stuttgart), Prof. Dr. Dr. h.c. mult. G. Wilke (Max-Pianck-lnstitut für Kohlenforschung, Mülheim/Ruhr) DIREKTOR (DIRECTOR) STELLVERTRETENDER DIREKTOR (DEPUTY DIRECTOR) Prof. Dr. Dr. h.c. Ekkehard Fluck Dr. W. Lippert HAUPTREDAKTEURE (CHIEF EDITORS) Dr. K.-C. Buschbeck, Ständiger Hauptredakteur Dr. H. Bergmann, Dr. H. Bitterer, Dr. H. Katscher, Dr. R. Keim, Dipl.-lng. G. Kirschstein, Dipi. Phys. D. Koschel, Dr. U. Krüerke, Dr. H. K. Kugler, Dr. E. Schleitzer-Rust, Dr. A. Slawisch, Dr. K. Swars, Dr. B. v. Tschirschnitz-Geibler, Dr. R. Warncke MITARBEITER (STAFF) Z. Amerl, D. Barthel, Dr. N. Baumann, I. Baumhauer, Dr. K. Beeker, Dr. W. Behrendt, Dr. L. Berg, Dipi.-Chem. E. Best, M. Brandes, E. Brettschneider, E. Cloos, Dipi.-Phys. G. Czack, I. Deim, Dipi.-Chem. H. Demmer, R. Dombrowsky, R. Dowideit, Dipi.-Chem.A. Drechsler, Dipi:-Chem. M. Drößmar, M. Engels, Dr. H.-J. Fachmann, Dr. J. Faust, I. Fischer, Dr. R. Froböse, J. Füssel, Dipl.-lng. N. Gagel, Dipi.-Chem. H. Gedschold, E. Gerhardt, Dr. U. W. Gerwarth, M.-L. Gerwien, Dipi.-Phys. D. Gras, Dr. V. Haase, H. Hartwig, B. Heibel, Dipi.-Min. H. Hein, G. Heinrich-Sterze!, H.-P. Hente, H. W. Herold, U. Hettwer, U. Hilberger, Dr. I. Hinz, Dr. W. Hoffmann, Dipi.-Chem. K. Holzapfel, Dipi.-Chem. W. Karl, H.-G. Karrenberg, Dipi.-Phys. H. Keller-Rudek, I. Knauss, Dipi.-Phys. E. Koch, Dr. E. Koch, Dipi.-Chem. K. Koeber, Dipi.-Chem. H. Köttelwesch, R. Kalb, E. Kranz, Dipi.-Chem. I. Kreuzbichler, Dr. A. Kubny, Dr. P. Kuhn, M. Langer, M.-L. Lenz, Dr. A. Leonard, Dipi.-Chem. H. List, H.Mathis, E. Meinhard, Dr. P. Merlet, K. Meyer, M. Michel, K. Nöring, C. Pielenz, E. Preißer, I. Rangnow, Dipi.-Phys. H.-J. Richter Ditten, Dipi.-Chem. H. Rieger, E. Rieth, Dr. J. F. Rounsaville, E. Rudolph, G. Rudolph, Dipi. Chem. S. Ruprecht, D. Schädle, V. Schlicht, Dipi.-Chem. D. Schneider, Dr. F. Schröder, Dipi. Min. P. Schubert, A. Schwärze!, Dipl.-lng. H. M. Somer, E. Sommer, Dr. P. Stieß, M. Teichmann, Dr. W. Töpper, U. Trautwein, Dipl.-lng. H. Vanecek, Dipi.-Chem. P. Velic, Dipl. lng. U. Vetter, Dipi.-Phys. J. Wagner, R. Wagner, Dipi.-Chem. S. Waschk, Dr. G. Weinberger, Dr. H. Wendt, Dr. B. Wöbke, K. Wolff, Dr. A. Zelle, U. Ziegler FREIE MITARBEITER (CORRESPONDENT MEMBERS OF THE SCIENTIFIC STAFF) Dr. I. Kubach, Prof. Dr. P. F. Linde, Prof. Dr. Y. Marcus, Dr. K. Rumpf, Dr. R. C. Sangster, Dr. R. P. Taylor, Dr. U. Trobisch EM. WISSENSCHAFTLICHES MITGLIED Prof. Dr. Dr. E. h. Margot Becke (EMERITUS MEMBER OF THE INSTITUTE) AUSWÄRTIGE WISSENSCHAFTLICHE MITGLIEDER Prof. Dr. Hans Bock (CORRESPONDENT MEMBERS OF THE INSTITUTE) Prof. Dr. Dr. Alois Haas, Sc. D. (Cantab.) Grnelin Handbook of lnorganic Chemistry 8th Edition u Uranium Supplement Valurne A4 Behavior of Uranium Fuels in Nuclear Reactors. Reprocessing of Spent Nuclear Fuels With 173 illustrations AUTHORS Helmut Aßmann, Kraftwerk Union AG, Erlangen Erich Merz, Kernforschungsanlage, Jülich Aristides Naoumidis, Kernforschungsanlage, Jülich Hubertus Nickel, Kernforschungsanlage, Jülich Heinz Stehle, Kraftwerk Union AG, Erlangen Gilbert N. Walton, Department of Chemical Engineering and Chemical Technology, Imperial College, London University, London, U.K. CHIEF EDITORS Kari-Christian Buschbeck, Gmelin-lnstitut, Frankfurt am Main Cornelius Keller, Supervising scientific coordinator for the Uranium Supplement Volumes, Schule für Kerntechnik, Kernforschungszentrum Karlsruhe System Number 55 Springer-Verlag Berlin Heidelberg GmbH 1982 LITERATURE CLOSING DATE: END OF 1979 IN MANY GASES MORE REGENT DATA HAVE BEEN CONSIDERED Library of Congress Catalog Card Number: Agr 25-1383 ISBN 978-3-662-06016-2 ISBN 978-3-662-06014-8 (eBook) DOI 10.1007/978-3-662-06014-8 This work is subject to copyright. All rights are reserved whether the whole or part of the material is concerned specifically those of translation, reprinting, re-use of illustrations, broadcasting, reproduction by photocopying machine or similar means, and storage in data banks. Under §54 of the German Copyright Law where copies are made for other then for private use, a Iee is payable to "Verwertungsgesellschaft Wort", Munich. © by Springer-Verlag Berlin Heidelberg 1981 Originally published by Springer-Verlag, Berlin · Heidelberg · New York 1981 Softcoverreprint of the hardcover8th edition 1981 The use of generat descriptive names, trade marks, etc. in the Gmelin Handbook, even if the !armer arenot especially identified, is not tobe taken as a sign !hat such names, as understood by the Trade Marksand Merchandise Marks Act, may according be used freely by anyone. Preface The present volume A4 of the "Uranium" series of the Gmelin Handbook deals with two very important technological aspects of the nuclear fuel cycle: - the behavior of fuel elements during burnup in a nuclear reactor, and - the reprocessing of spent fuel to recover the non-fissioned uranium and newly created materials. The usefullifetime of a fuel element in a nuclear reactor depends strongly on the change of its chemical and physical properties during irradiation. Properties like thermal conductivity, swelling, creep, and oxygen-to-metal ratio are strongly affected by the intense neutron field and the energetic fission products. Furthermore, the high temperature gradient in a fuel element also produces alterations of the initial fuel. such as densification or U: Pu segregation. All of these effects are thoroughly discussed for the different kinds of fuels to be used in modern nuclear reactors today or in the future. The vast amount of very often Contradietory results in sometimes difficultly obtainable Iiterature has been summarized to create a compendium in this field with the two sections, on oxide and on carbide and nitride fuels, respectively. The chapters on reprocessing of spent fuels deal only with fuel elements of the uranium thorium fuel cycle and with those containing fuel highly enriched in 235U. The treatment of U02 and (U,Pu)0 has already been given in the transuranic element series. 2 Due to the vast amount of Iiterature published within the topics of this book, only selected and important papers have been mentioned here. For other references see the "General References" etc. in this book. The Iiterature is evaluated for the period up to the end of 1979, in many cases more recent Iiterature has been considered. I thank the authors from industry and the nuclear research centers for their excellent collaboration. I thank also the Gmelin Institute, with Prof. Dr. Y. Marcus, who translated the originally German text into English, Dr. K. C. Buschbeck as the supervising editor and Prof. Dr. Dr. h.c. E. Fluck as director, for its support and encouragement. Frankfurt am Main December 1981 Cornelius Keller Table of Contents Page 1 The Behavior of Uranium Fuels in Nuclear Reactors. 1.1 Oxide Fuels . . 1 lntroduction and Survey 3 1.1.1 Effects of the Fission Fragments in the Crystal Lattice 5 Properties of the Fission Fragment Spike . . 5 lncreased Seit-Diffusion . . . . . . . . . . 8 Formation and Annealing of Lattice Defects . 8 1.1 .2 Mechanical Behavior . . . . . . . . . 11 Elastic Behavior. . . . . . . . . . . . . . 11 Plastic Behavior and Behavior upon Fracture 12 Creep Behavior . . . . 14 Theoretical Models . . . . . 17 Experimental Results . . . . 19 Primary and Transient Creep . 26 1.1.3 Thermal Behavior. . . . . 29 Thermal Conductivity and Conductivity Integral of U02. 29 Experimental Results . . . . . . . . . . . . . . . 30 Thermal Expansion and Specific Heat Capacity. . . . . 35 1.1 .4 Behavior of the Fission Products and Release of Fission Gases 39 Concentration of the Fission Products. 40 Solid and Volatile Fission Products . . . . . 40 Fission Products in the Fuel . . . . . . . 41 The Behavior of Volatile Fission Products . 44 Behavior of the Fission Gases in the Fuel 45 The Formation and Growth of Bubbles 46 Bubble Migration ..... 48 The Release of Fission Gases .. 50 Experimental . . . . . . . . 50 Models for Low Tamperatures 50 Models for Intermediate Tamperatures 51 Model for High Tamperatures .... 63 The Diffusion Coefficient of Fission Gases 64 1.1.5 Changes in Dimensions lnduced by Irradiation (Densification and Swelling) . 70 lrradiation-lnduced Densification . . . . . . . . . . . . . . . . . . . . . . . 71 Theoretical Models for Thermally Activated and lrradiation-lnduced Densification 71 Experimental Studies . . . 77 Swelling by Fission Products. . . . 80 Experimental Results . . . . . . 80 Mechanistic and Empirical Models 84 The Superposition of Swelling, Densification, and Other Deformative Phenomena . 86 II Page 1.1 .6 Restructuring. . . . . . . . . . . . . . . . . 92 Phenomenological Description of the Structural Zones 92 Crack Patterns and Relocation 95 Grain Growth. . . . . 98 Theoretical Models . . . . 98 Experimental Results . . . 99 Pore Migration, Columnar Grain Growth, Central Void 102 1.1.7 Changes in the Stoichiometry, Redistribution of Oxygen and Uranium/ Plutonium . . . . . . . 106 Thermodynamic Data Base. . 107 Changes in the Stoichiometry 110 Fuel in Steel Cladding. . 110 Fuel in Zircaloy Cladding . 112 Redistribution of Oxygen . . 112 Redistribution of Uranium and Plutonium in a Mixed Oxide. 118 1.1.8 Interaction with the Cladding .. 123 lnterior Corrosion in Zircaloy Cladding 124 lnterior Corrosion in Steel Cladding. . 124 Cooperative Mechanical and Chemical lnteractions. 126 Mechanical Interaction between Fuel and Cladding 126 Stress Corrosion Cracking (SCC) Arising from Pellet/Ciad Interaction (PCI) 127 1.1.9 Behavior of Oxidic Nuclear Fuels in Defective Fuel Rods. 135 Water Cooled Fuel Elements . 135 Sodium Cooled Fuel Elements . . . . . . 137 1.2 Carbide and Nitride Nuclear Fuels. 139 1.2.1 lntroduction . . . . . . . . . . . . 139 1.2.2 Properties in the Non-lrradiated State 142 Mechanical Properties . 143 Creep Behavior . . . . . . 143 Carbides ....... . 143 Nitrides, Carbide Nitrides 146 Elastic Properties 148 Strength . . . . 150 Hardness .... 151 Thermal Properties 153 Coefficient of Thermal Expansion. 153 Carbides ....... . 153 Nitrides, Carbide Nitrides 154 Thermal Conductivity 156 Carbides. 156 Nitrides .... . 160 Diffusion ...... . 164 Seit-Diffusion in Uranium Carbides. 164 Effect of the Composition on the Diffusion of Uranium. 165 III Page Effect of lmpurities on the Diffusion of Uranium. 166 Effect of Nitrogen on the Diffusion of Uranium 167 Diffusion of Other Actinides in Carbides . . . 167 The Contribution of Grain-Boundary Diffusion 168 Diffusion of Carbon in Carbides . . . . . . . . 169 The Effect of Nitrogen on the Mobility of the Carbon 170 Self-Diffusion of Metal Atoms in Nitrides. . . . . 170 Diffusion of Nitrogen in Nitrides . . . . . . . . . 171 Diffusion of Fission Gases in Carbides and Nitrides 171 Electrical Resistivity . 175 Carbides . . . . . . . . . . . . 175 Nitrides . . . . . . . . . . . . 177 Compatibility with Metallic Materials 180 Compatibility of Carbidic Fuels and Breeding Materials with Austenitic Steels 180 Compatibility of UC with Other Metallic Materials . . . . 184 Compatibility of (U,Pu)C with Various Cladding Materials 185 Compatibility of Nitride Fuels with the Cladding. 187 Compatibility of Uranium Carbide Nitrides. . . . . . . . 188 1 .2.3 Irradiation Behavior. . . . . . . . . . 191 Changes in the Physical Properties . . . . . 191 lrradiation-lnduced Creep Processes in UC and UN 191 Irradiation Effects on Diffusional Processes 192 Change of the Hardness on Irradiation 193 Changes ofThermal Conductivity . 194 Changes of the Electrical Resistivity 195 In-Pile Compatibility. . . . . . . . . 196 Carbide Fuels. . . . . . . . . . . 196 Results of Irradiation of UC with Cr-Ni Steels. 197 UC with Tungsten . . . . . 198 UCwithNb-1%Zr..... 198 (U,Pu)C with Stainless Steel 198 (U,Pu)C with Nb-1% Zr 201 Nitride Fuels . . . . . . . 201 lrradiation-lnduced Swelling . 204 Uranium Carbide . . . . . 204 lrradiation-lnduced Swelling of (U,Pu)C Mixed Carbides. 209 Nitride and Nitrogen-Containing Carbide Fuels: UN, U(C,N). (U,Pu)N, and (U,Pu)(C,N) . . . . . . . . . . . . . . . . . . . . . 214 Mechanism of the Swelling of Carbide and Nitride Fuels . 218 The Release of Gaseous Fission Products . 227 Mechanisms of the Fission Gas Release. . . . . . . . . 227 Fission Gas Release from UC . . . . . . . . . . . . . 228 The Temperature Dependence of the Fission Gas Release from UC 228 Effect of the Stoichiometry on the Fission Gas Release from UC 230 Effect of the Porosity and the Microstructure . 231 Effect of the Burnup and of the Power Density 233 Fission Gas Release from (U,Pu)C . . 234 Fission Gas Release from Nitride Fuels . . . . . 241
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