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The Reaction Between Iodine and Silver Under Severe PWR Accident Conditions

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The Reaction Between Iodine and Silver Under Severe PWR Accident Conditions 283 '"" CH9700209 The Reaction between Iodine and Silver under Severe PWR Accident Conditions. An Experimental Parameter Study. F. Funke, G.-U. Greger, A. Bleier, S. Hellmann, W. Morell Abstract An extensive experimental parameter study was performed on the kinetics in the reaction systems k/Ag and F/Ag in a laboratory-scale apparatus. Starting with h or F solutions and silver powder suspensions, the decrease of soluted t or F, respectively, due to fixation on the silver particles, was monitored as function of time using the radioactive tracer 1-131. The measured data were analyzed using a model of first order kinetics with respect to the iodine concentration. However, the analysis using first order kinetics had to be performed separately in an early, fast reaction phase (0-5 min) and in a late, slow reaction phase (5-30). The reason for this unexpected behaviour was not identified. Thus, rate constants, two for each test, were deduced from 14 VAg main tests and from 36 F/Ag tests. No dependencies of the rate constants were found on the parameters temperature (varied between 25°C and 160°C), pH (3-7), initial iodine concentration (1E-4-1E-6 mol/1), presence of boric acid (2000 ppm), type of silver educt (different powders, plate, coarse shreddings of control rod material), and pretreatment of the silver educt (hydrogen reduction) prior to the tests. However, the stirring of the reaction solution generally enhanced the kinetics highlighting the importance of mass transfer. The F/Ag reaction proceeded only if there was no inertization of the reaction solution by sparging with nitrogen. The temperature-independent rate constant for the early, fast fe/Ag reaction phase is 2E-5 m/s. However, a smaller rate constant of 6E-6 m/s is recommended for use in source term calculations with IMPAIR, which already contains a first order model. Analogeously, the temperature-independent F/Ag reaction rate constant is 8E-6 m/s in an early, fast reaction phase. For use in source term calculations, a smaller rate constant of 2E-6 m/s is recommended. The lower bound of the F/Ag rate constant was 3E-8 m/s which could be used in very conservative source term calculations. If there is a boiling sump, and neglecting oxidation effects due to radiation, inertizing conditions would be more appropriate to the F/Ag system and in this case the F/Ag reaction should be switched off. Inconsistencies in the literature data on the solubilities of silver iodide at high temperatures were clarified experimentally. The solubility of stoichiometric Agl suspended in water at T=160°C was measured by taking several samples from the homogenous solution and amounts to 1.3E-5 mol/1. This value fits well with the majority of the literature data in an Arrhenius type representation. The data of this work are helpful in quantifying the effect of silver iodide as an iodine sink in LWR severe accidents. All authors: Siemens AG, Power Generation Group (KWU), D-91050 Erlangen, P.O. Box 3220, F. R. Germany 284 1. INTRODUCTION The knowledge of the chemical behaviour of radioiodine in the containment during a hypothetical core melt accident is essential for the prediction of the source term to the environment using available iodine codes. An important aspect so far not sufficiently contained in the modelling arises from the presence of large amounts of silver in PWR silver/indium/cadmium control rods. The chemical reaction between iodine and silver leads to the formation of non-volatile silver iodide. Consequently, this reduces the iodine volatility or even represents a permanent iodine sink in PWR severe accidents, provided that silver iodide is stable against radiation. Due to its high volatility at core melt temperatures, silver (Ag) is evaporized and can reach the containment sump. The Ag inventory in a PWR exceeds that of iodine by up to a factor of 100 and therefore even small quantities of silver reaching the sump represent a significant reaction partner for iodine. A literature study showed that Ag particles in the aqueous phase react with molecular iodine Cb) and with iodide ions (T) by formation of silver iodide (Agl) layers on the Ag particles surfaces. Agl has a very low solubility in water and is non-volatile under severe accident containment boundary conditions. Provided furthermore that it withstands radiolytic disintegration, Agl represents a permanent iodine sink. It is therefore essential to model the aqueous silver/iodine chemistry in severe accident iodine codes taking into account parameters in the sump boundary conditions that have to be identified experimentally. The present knowledge on the silver/iodine reaction indicates that Agl layers on the Ag particles are formed by reaction of Ag particles with I2 and with water-soluble iodide T. However, it is not clear from published literature, how boundary conditions in the sump water such as pH, temperature etc. influence the formation of low-soluble Agl. Additionally, there are uncertainties in the literature on the solubility of Agl in water at high temperatures up to 160°C. Due to lacking information on these questions, the influence of silver on the iodine volatility under severe accident containment conditions can therefore not adequately be modeled in the existing iodine codes (INSPECT, IODE, IMPAIR, LIRIC). An experimental parameter study was therefore performed in order to create a data basis which allows an improved modeling of the silver/iodine chemistry in severe accident iodine codes. 285 2 EXPERIMENTAL 2.1 Principle The experiments on the kinetics in the reaction systems h or I~ with silver were planned in order to clearly define boundary conditions kept fixed during the tests and to take various samples out of the reaction mixture during the tests without interupting them. Remark: throughout the whole paper we use the expression iodine as representing in general all different iodine species. Instead, in cases where the chemical symbols are used (I2 for elemental iodine or T for iodide in aqueous solution) a distinction between the various iodine species is necessary. 2.2 Apparatus Tests at T < 100°C were performed in the apparatus shown in the Figure 1. A glass vessel with 12 cm inner diameter and 20 cm height contained the reaction suspension consisting of small silver particles and aqueous iodine solution. The vessel was placed on a magnetic stirring hot plate. The cover is equipped with a sampling line, a thermometer, a cooler, and a separatory glass funnel for dosing of the silver suspension at the beginning of each test. A second vessel besides the reaction vessel originally contained a sodium hydroxide solution and serves to collect the reaction suspension at the end of each test. This second vessel is equipped with a security valve. Tests at T = 160°C were performed essentially in the same way as for lower temperatures, but a glass autoclave was employed as reaction vessel. Dimensions and equipment were essentially very similar to those of the apparatus for T<100°C tests. 2.3 Method A standard method was developed in the course of the experiments and is described in the following. An aqueous solution (1 liter) of either I2 or T was brought to a defined pH in the reaction vessel. Iodine tracer acitivity (usually about 4E6 Bq 1-131) was added. A suspension of silver powder (10 ml water with adjusted pH and containing lg Ag) was prepared and filled into the separatory funnel. A supersonic pretreatment of the silver/water mixture was performed prior to the test to destroy agglomerates and to prevent whirl-up of silver particles onto the surface of the suspension. In some tests, silver plates were used instead of silver powder. Tests were initiated by the addition of the silver suspension to the iodine solution within 30 seconds. In most tests the suspension was stirred. Durations of the tests were up to 300 minutes. Samples were usually taken after 2 min, 5 min, 10 min, 20 min, 30 min, 60 min, 120 min, 200 min and 300 min to determine the amount of unreacted iodine. Shortly before each sampling the stirrer was switched off in order to let the silver particles be deposited on the bottom of the reaction vessel and to be able to take samples out of the homogeneous aqueous solution (without Ag or Agl-coated Ag particles). Additionally, the samples were filtered above glass filters to remove Agl coated particles. The remaining 1-131 activity of the sample, being representative for the unreacted iodine concentration in the rection vessel, was measured. At the end of each test, the reaction suspension was transferred into the second vessel where I2 in the aqueous phase was reduced to non-volatile F by NaOH. The suspension was filtered 286 and the filter content was washed with Na2S2C>3 to redissolve the iodine on the Agl particles. The 1-131 measurement of this washing solution yielded the iodine loading on the Ag particles. 2.4 Test matrix A large number of parameters was variied in the tests as described below The complete test matrices are given in Table 1 (main tests in the WAg system), Table 2 (pre-tests in the 17Ag system) and Table 3 (main tests in the T/Ag system). It was found during the course of the programme that the pre-tests in the F/Ag reaction system yielded data of the same quality as in the following main tests and consequently, the pre-test data were included in the analysis of the parameter study. Five different stiver educts were used: • fine powder with 2.0 - 3.5 ^m diameter, 0.2 m2/g specific surface, delivered by Aldrich, • fine powder with 2.0 - 3.5 um diameter, 0.34 m2/g specific surface, delivered by Johnson- Matthey, • 60 mesh powder, 0.13 m2/g specific surface, delivered by Aldrich, • coarse shreddings of silver/indium/cadmium control rod material, total surface = 0.186 m2, • silver metal sheet, total surface = 0.01 m2.
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