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ATOMIC ENERGY F F S L'energie ATOMIQUE of CANADA UMITED T AECL-6f)2 ATOMIC ENERGY ffS L'ENERGIE ATOMIQUE OF CANADA UMITED Tif T DU CANADA UMITEE ASSESSMENT OF IODINE BEHAVIOUR IN REACTOR CONTAINMENT BUILDINGS FROM A CHEMICAL PERSPECTIVE EVALUATION DU COMPORTEMENT CHIMIQUE DE L'lODE DANS L'ENCEINTE DE PROTECTION D'UN REACTEUR Robert J. Lemire', Jean Paquette, David F. Torgerson , David J. Wren1, J. Wallace Fletcher2 Whiteshell Nuclear Research Establishment Etablissement de Recherches Nucle'aires de Whiteshell * Chalk River Nuclear Laboratories Laboratoires Nucleaires de Chalk River Whiteshell Nuclear Research Etablissement de Recherches Establishment Nucle'aires de Whiteshell Pinawa, Manitoba ROE 1L0 June T981 juin ATOMIC ENERGY OF CANADA LIMITED ASSESSMENT OF IODINE BEHAVIOUR IN REACTOR CONTAINMENT BUILDINGS FROM A CHEMICAL PERSPECTIVt by Robert J. Lemire , Jean Paquette , David F. Torgersor) , 1 2 David J. Wren and J. Wallace Fletcher Research Chemistry Branch Whiteshell Nuclear Research Establishment Physical Chemistry Branch Chalk River Nuclear Laboratories Whiteshell Nuclear Research Establishment Pinawa, Manitoba ROE 1L0 1981 June AECL-6812 EVALUATION DU COMPORTEMENT CHIMIQUE DE L'IODE DANS L'ENCEINTE DE PROTECTION D'UN REACTEUR par Robert J. Lemire , Jean Paquet te , David F. ïorgerson , 1 2 David J. Wren et J. Wallace Fletcher RESUME Les paramètres thermodynamiques pour les espèces aqueuses, solides et gazeuses de l'iode à 25°C ont été obtenus à partir d'un examen de la littérature chimique. Ces données ont été rendues com- patibles avec la compilation du groupe CODATA. En utilisant les données thermodynamiques à 25°C, les valeurs de l'énergie libre de formation ont été évaluées en fonction de la température, jusqu'à 150°C, et ce pour toutes les espèces de l'iode. Les résultats sont présentés sous forme de diagrammes tension-pH, de diagrammes cîe distribution d'espèces et de coefficient de partage phase liquide/phase gazeuse. On discute aussi de la chimie de l'iode à l'intérieur même du combustible nucléaire, dans le circuit de refroidissement primaire et dans l'atmosphère de l'enceinte de protection. Cet examen du comportement chimique de l'iode démontre clairement qu'il est possible de I.xmiter la concentration de l'iode dans l'atmosphère de l'enceinte de protection, iode pouvant être libéré à la suite d'une perte accidentelle de fluide refroidisseur durant laquelle le combustible nucléaire serait endommagé. Service de la Recherche Chimique Etablissement de Recherches Nucléaires de Whiteshell Service de la Chimie-Physique Laboratoires Nucléaires de Chalk River L'Energie Atomique du Canada Limitée Etablissement de Recherches Nucléaires de Whiteshell Pinawa, Manitoba ROE 1L0 1981 juin AI :L-6812 ASSESSMENT OF IODINE BEHAVIOUR IN REACTOR CONTAINMENT BUILDINGS FROM A CHEMICAL PERSPECTIVE by Robert J. Lemire , Jean Paquette , David F, Torgerson , 1 2 David J. Wren and J. Wallace Fletcher ABSTRACT Thermodynamic parameters for aqueous and gaseous iodine species at 25°C have been obtained from the literature and a data base has been constructed that is consistent with CODATA values. Using the 25°C data base, Gibbs energies for the iodine species have been calculated as a function of temperature to 150°C. Results are presented in terms of potential/pH diagrams, species distribution diagrams, and liquid/gas partition-coefficient plots. Iodine chemistry in the fuel, in the primary coolant system, and in the containment building atmosphere is also discussed. This assessment of iodine behaviour clearly shows that there is considerable scope for limiting the concentration of airborne iodine in reactor containment buildings following a loss-of-coolant accident in which fuel failure occurs. Research Chemistry Branch Whiteshell Nuclear Research Establishment Physical Chemistry Branch Chalk River Nuclear Laboratories Atomic Energy of Cpnada Limited Whiteshell Nuclear Research Establishment Pinawa, Manitoba ROE 1L0 1981 June AECL-6812 CONTENTS Page 1. INTRODUCTION 2. IODINE CHEMISTRY IN THE FUEL 3. IODINE CHEMISTRY IN THE PRIMARY SYSTEM 3 3.1 DISCUSSION 3 3.2 SUMMARY 5 IODINE SOLUTION CHEMISTRY IN THE CONTAINMENT 4.1 INTRODUCTION 5 4.2 SOLUTION SPECIES 6 4.3 IODIKE VOLATILITY 11 4.4 DISTRIBUTION DIAGRAMS 12 4.5 GAS-LIQUID PARTITION COEFFICIENTS 13 4.6 KINETIC FACTORS INFLUENCING IODINE SPECIATION IN AQUEOUS SOLUTION 15 4.7 HYDRAZINE REACTIONS 18 4.8 SUMMARY 20 5. GAS PHASE BEHAVIOUR 21 .5.1 INTRODUCTION 21 5.2 GAS PHASE REACTIONS 22 5.2.1 Inorganic Iodine 22 5.2.2 Methyl Iodide 23 5.3 IODINE SURFACE ADSORPTION AND DESORPTION 24 5.4 SUMMARY 26 6. CONCLUSIONS 26 REFERENCES 28 .../cont. CONTENTS, concluded Page TABLES 33 FIGURES 36 APPENDIX A SUMMARY OF LARGE-SCALE TESTS - IODINE IN CONTAINMENT 47 APPENDIX B THERMODYNAMIC DATA 57 APPENDIX C FACTORS AFFECTING SURFACE ADSORPTION AND DESORPTION OF IODINE 70 1. INTRODUCTION The objective of this report is to assess iodine behaviour in nuclear reactor containment buildings and to identify the key areas for further research that could lead to improvements in the analysis of iodine emissions. For postulated loss-of-coolant accidents (LOCA) where fuel failure occurs, it has usually been assumed that a large fraction of the iodine released from fuel becomes airborne in the containment building and is, therefore, available for release to the environment. However, iti the Three Mile Island accident, even though a high percent- age of the iodine inventory in the reactor core was released, airborne iodine concentrations were small . This emphasizes the complex behav- iour of this element but, more importantly, it shows that we have an opportunity to identify processes that could be effective for iodine abatement in CANDU systems. Figure 1 traces possible iodine behaviour if it is released from the fuel as Csl into a reducing steam environment. The broken line represents the interface between the primary coolant system and con- tainment. The boxes represent the various chemical and physical forms of iodine. In general, iodine can change from one form to another as indicated by the arrows. If Csl encounters different conditions in the primary system, the iodine species released to the containment will change and their subsequent behaviour will change accordingly. An important observation from Figure 1 is that both the gas phase and the solution phase are important in iodine behaviour. There are a number of "sinks" in both phases that could tie up the radioiodine until it decays, and these are marked in the upper right-hand corner of the appropriate boxes. Previously, the solution "sinks" have not been effectively assessed in accident analysis and it has been assumed that a large fraction of the iodine is available for release from the contain- ment. Therefore, in this work, we have concentrated on a better - 2 - characterization of the behaviour of iodine in aqueous solutions under LOCA conditions. Because of the complex behaviour of iodine, we have used predictive methods based on thermodynamic and chemical kinetic informa- tion to analyze the overall problem and to evaluate the sensitivity of various parameters. In this way, a fundamental understanding of a relatively few key parameters has led to an improved assessment of the overall system and allowed us to focus on the important measurements. 2. IODINE CHEMISTRY IN THE FUEL The chemistry of iodine within the fuel is controlled by thermodynamic equilibria. At fuel operating temperatures, rates of (2 3) solid-state reactions are limited by diffusion ' . Based on experi- mentally measured fission-product releases, the assumption that the fission products are produced isotropically within the fuel appears justified, permitting equilibrium calculations. On this basis, therroo- dynamic equilibrium calculations have been made by Pobereskin et al. (3) and Besmann and Lindemer . The controlling parameter of the chemistry in the fuel is the oxidation potential (uQ ). Cubicciotti et al. have calculated that, at the normal oxidation potentials in fuel, cesium uranates are formed, and Besmann and Lindemer have shown that UQ is primarily controlled by the reaction between UO and Cs?UO . CANLUB graphite lubricant inside the fuel sheath may act as a reducing agent to maintain a low oxidation potential, but this has not been investigated in thermodynamic calculations. The large excess of cesium over iodine (Cs:I -v. 10:1) and the high stability of Csl result in Csl being the most stable form of iodine at low fuel oxidation poten- tials • . The existence of iodine as Csl in fuel has been demon- strated experimentally by Lorenz et al. - 3 - While Csl is the major form of iodine, Zrl, and Zrl,, both volatile at fuel temperatures, may exist at concentrations several (3) orders of magnitude lower than Csl . The high radiation fields will disturb the thermodynamic equilibria and very small steady-state concen- trations of I, and of I atoms will also be present. There is no direct evidence that organic iodides exist in measureable quantities in the fuel. 3. IODINE CHEMISTRY IN THE PRIMARY SYSTEM 3.1 DISCUSSION The chemistry of iodine within the primary coolant system is extremely complex, owing to the high temperatures, radiation fields, and a variety of oxidation potential conditions. Reaction rates will be rapid although thermodynamic equilibrium may not be attained in cases where residence times are short. Iodine is probably released to the primary system as vapour phase Csl and subsequent reactions depend on the conditions encountered. As summarized in Figure 1, the following conditions or any combination thereof may prevail: 1. Reducing or mildly oxidizing steam. Csl is stable to at least 1600°C under these conditions . Below ^ 1300°C, Csl will plate out on surfaces a"d will only be removed if oxygen or liquid H,0 is present. If the steam/CsI mixture is condensed, iodine will be converted to I (aq). 2. Steam/air. Under oxidizing conditions, Csl may rapidly react with 0, to form CS2O and I2. Cso0 and I^O will further react to form CsOH.
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