Nuclear Engineering and Design 191 (1999) 53 67 www.elsevier.

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Experiments and computational models for aerosol behaviour in the containment

K. Fischer *, T. Kanzleiter
Battelle Ingenieurtechnik GmbH, Dusseldorfer Strasse 9, 65760 Eschborn, Germany Received 20 November 1998; accepted 23 February 1999

Abstract Aerosols generated by condensation of volatile ssion products during nuclear reactor core meltdown accidents represent a major fraction of the accidental airborne radioactivity. A comprehensive experimental research programme was performed at Battelle to investigate the transport and deposition behaviour of aerosols in the containment, in order to support the development of computer models which estimate the ssion product behaviour in the containment and the source term for potential radionuclide releases to the environment. Important steps in the investigations were: (1) DEMONA experiments. The rst large scale aerosol test series performed in the Battelle model containment (BMC) (total volume 640 m3), using an open (quasi one-room) geometry and condensation aerosols from a plasma torch generator. (2) VANAM experiments. Advanced aerosol tests in the BMC, using a multi-room geometry, mixed hygroscopic/non hygroscopic condensation aerosols, a double injection period, and varying thermohydraulic conditions. One of the experiments was subject of the International Standard Problem ISP 37. (3) KAEVER experiments. A systematic investigation of aerosol materials and mixtures and the related deposition behaviour, using a simplied one-room test vessel (10 m3 volume) and advanced instrumentation. Important computer codes developed and/or validated in connection with the experiments are FIPLOC and NAUA; aerosol codes CONTAIN, MELCOR and GOTHIC-MAEROS were also applied. Some important results from the investigations and code developments are: (1) signicant local aerosol concentration differences can occur in a multi-room geometry; (2) concentration differences can be caused by atmospheric stratication; and (3) deposition is strongly affected by material hygroscopicity and atmospheric humidity. (4) Satisfactory prediction requires a consistent treatment of multi-room thermal hydraulics, aerosol transport and steam condensation on particles. (5) Prediction results can be affected by numerical stability and nodalization (user experience). This paper presents a number of results of the experimental investigations and the present state of code modelling, with special reference to the ndings of ISP37. 1999 Elsevier Science S.A. All rights reserved.

1. Introduction
 Paper presented to the Post-SMIRT Seminar Aerosols in the Containment, 25 26 August 1997, Saclay, France. * Corresponding author. Tel.: +49-6196-93616; fax: +496196-936399.

During a nuclear reactor core meltdown accident, radioactive ssion products are released from the fuel elements and carried into the con-

0029-5493/99/$ - see front matter 1999 Elsevier Science S.A. All rights reserved. PII: S 0 0 2 9 - 5 4 9 3 ( 9 9 ) 0 0 0 5 2 - 7

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tainment. In order to assess the potential radioactivity releases from the containment to the environment, the behaviour of the ssion products in the containment must be known. Since most of the important radionuclides are present in the form of aerosols, aerosol deposition on internal surfaces can reduce the release of radioactivity. Furthermore, the release of radioactivity may be affected by local aerosol concentrations near the leak position. Computational models for aerosol behaviour in the containment atmosphere are generally based on models for the atmosphere thermal hydraulics, giving information on pressure, temperature, humidity, water distribution, and possibly atmospheric ow circulations and volumetric leak rates. The behaviour of the aerosol particles, like agglomeration, deposition on walls, and advective transport, is dependent upon the thermal hydraulic conditions in many aspects. Aerosol source terms to the containment atmosphere are provided by other models, e.g. models for ssion product transport in the primary system or models for aerosol generation in the reactor cavity after failure of the reactor pressure vessel. Early model developments for containment thermal hydraulics and aerosol behaviour were based on the assumption of homogeneous conditions in the containment. Similar ideas were followed when rst experiments were conducted to provide data for code validation. At later stages, research into a more detailed understanding of thermal hydraulic phenomena, especially the question of hydrogen gas distribution, made it clear that strongly inhomogeneous conditions can develop within a largescale containment. A new generation of codes was developed that was designed to simulate the inhomogeneous distributions, and corresponding experimental work was performed. The present paper gives a brief overview of the experimental and theoretical developments, including a summary of achievements and open issues.

tive for many others that perform similar model calculations.

2.1. NAUA
The NAUA code (Bunz et al., 1983) was developed at KfK around 1983. It simulates coagulation, sedimentation, diffusional deposition and steam condensation on particles. The code uses a numerical representation of the particle size distribution. Thermal hydraulic data must be supplied as input to the code. Simulations are done for a single control volume, where aerosol sources and leaks are taken into account. An extension of the original version is NAUA Mod 5-M (Bunz et al., 1987) for multicompartment geometries, where the NAUA aerosol simulations are performed for several control volumes. In addition, advective ows between different control volumes are taken into account. Thermal hydraulic conditions and intercompartment ow rates have to be specied as input data. Thus, NAUA requires the operation of an extra code for containment thermal hydraulics, and does not take into account possible feedback effects which aerosols may cause in the thermal hydraulic conditions. An extension to the NAUA code called NAUAHYGROS was developed by Jokiniemi, in order to take into account the effects of hygroscopic aerosols during steam condensation (Jokiniemi, 1990).

2.2. FIPLOC
The FIPLOC code (Weber et al., 1996) was developed by GRS. Starting with a lumpedparameter model for multi-room containment thermal hydraulics (RALOC, Jahn et al. (1986)), the aerosol code MAEROS (Gelbard, 1991) was integrated and extended. The aerosol model MAEROS has similar features as NAUA, but it uses a more advanced numerical solution scheme, which allows to work with less particle size classes and reduced numerical effort. The coupled system FIPLOC-MAEROS calculates the thermal hydraulics of a multicompartment geometry, taking into account possible feedback effects caused by

2. Computational models In the following, a limited number of aerosol codes will be discussed; these codes are representa-

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aerosols; it calculates aerosol coagulation and deposition in each control volume, and advective ows between different volumes. Steam condensation on aerosol particles is simulated, and hygroscopic effects can be taken into account.

2.3. CONTAIN and MELCOR

The codes CONTAIN (Murata et al., 1989) and MELCOR (Summers et al., 1994) were both developed by Sandia National Laboratories for the US NRC. While CONTAIN is a bestestimate code for containment analysis including reactor cavity phenomena, MELCOR is designed as an integrated code for severe accident analysis, including models for the containment, the primary system and the degraded core. Both codes have features similar to FIPLOC, making use of a multi-compartment lumped-parameter representation of the containment and using MAEROS as the basic aerosol simulation model. Some differences exist in the implementations of the thermal hydraulic and aerosol models that will be discussed below.

2.4. Discussion of models

In a coupled thermal/hydraulic-aerosol model with multicompartment capability, aerosols can be considered in a rst-order approximation as tracer substances that are transported between the compartments by the advective ow velocities calculated in the thermal/hydraulic model part. Agglomeration acts as a mass transfer mechanism between aerosol size classes, and deposition acts like a sink term to the airborne aerosol concentrations. The aerosols may be represented by a certain number of size classes ( 10 20 in MAEROS, 50100 in NAUA). In addition, different material compositions (e.g. radionuclide species) may be accounted for. In a typical MAEROS application, 20 size classes and three material species (non-hygroscopic, hygroscopic and water aerosol) lead to 60 dependent variables per computational zone that must be computed in addition to the thermal hydraulics. Advective

aerosol transport over vertical ow paths interferes with the sedimentation velocity of the particles. Since this velocity depends upon the particle size, the effective aerosol transport velocity can be considerably higher than the gas velocity, especially for larger particles. A separate control of the material Courant number for the different aerosol size classes must be established to avoid numerical problems. Steam condensation on aerosols has a major impact on the overall deposition rate. In order to achieve a consistent model for steam condensation on aerosols, the following effects must be taken into account: steam and gas sources and sinks, intercompartment ows; heat transfer rates to walls; steam condensation on walls; evaporation; gas pressure and temperature; and steam transfer to aerosol particles, and removal of condensation heat. By means of a mass and energy balance of the atmosphere in a computational zone, a thermodynamic state can be determined which is generally different from thermal equilibrium or saturation. If the result is super-saturated, the amount of steam that exceeds the saturation concentration can be considered as fog formation mass because equilibrium conditions are achieved within seconds, as determined by Masons rate equation. Particle growth in super-saturated steam is affected by the Kelvin effect resulting from the surface tension of the aerosol droplets and the corresponding equilibrium steam pressure on the surface of the droplets. Due to this effect, a critical droplet size exists, with droplets of smaller size being unable to grow under given supersaturation conditions. A major part of the aerosols from a core meltdown accident is hygroscopic, especially due to CsI and CsOH components. Steam is condensed on hygroscopic aerosols even under superheated atmospheric conditions, and release of hygroscopic particles can increase the superheating. Modeling steam condensation on hygroscopic aerosols requires a consistent simultaneous treatment of heat and mass balances including the

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aerosol water steam exchange in each computational zone. This is much more complicated than modeling steam condensation on non-hygroscopic aerosols, the latter being a pure thermodynamic calculation without any feedback from the aerosol behaviour. Two more coupling effects between aerosol and thermal hydraulics shall be mentioned. One is the change in atmospheric density introduced by high concentrations of aerosols, which may give rise to natural convection currents. The other is associated with the release of decay heat from aerosol particles, either suspended or deposited on walls or in pools. The heat from b- or g-ray emissions can introduce natural convection currents; it may enhance the superheating of the atmosphere and thus reduce the potential for steam condensation on aerosols; on the other side, decay heat release may lead to evaporation of water from droplets, water lms and pools, thereby increasing the atmospheric saturation and the potential for steam condensation on aerosol particles. Numerical problems are often encountered when modeling the coupled thermal hydraulic/ aerosol dynamics, because of some highly transient processes occurring during steam

condensation on aerosols. A well balanced method of discretisation in space and time and appropriate iterations for intercompartment ows, zone-internal processes and heat exchanges with structural walls has to be established for to obtain meaningful results. The following discussion of experiments and associated code validations shall indicate the present state of modeling and the still open questions.

3. Experiments and code validations

3.1. DEMONA
The DEMONA aerosol containment experiments (Liljenzin et al., 1990) were conducted in the Battelle model containment (BMC), a cylindrical test facility of 640 m3 volume with subcompartments and concrete walls. Fig. 1 shows the arrangement used for the DEMONA test series. Aerosols were generated by plasma torch generators and injected directly into the central subcompartment. By optional injection of steam, the atmospheric humidity and the related condensation processes could be varied. Tests were con-

Fig. 1. DEMONA test facility.

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Fig. 2. Measured aerosol mass concentrations during DEMONA tests B2 (dry), B3 and B4 (wet).

ducted with different aerosol materials: tin oxide, iron oxide, silver and mixtures of tin oxide with iron oxide. Instrumentation was provided to measure atmospheric pressure, temperature distribution of atmosphere, sump water and walls, relative humidity, heat transfer rates, injection rates and temperatures, and the concentration of injected tracer gas for leakage control. Aerosol and droplet concentrations and particle size distributions were determined by lters, impactors, photometers, a spectrometer and calorimeters. For the majority of tests, most vents were opened to enable rapid mixing and homogeneous conditions. Table 1 shows the test matrix. In experiment A9, a number of vent connections was closed, in order to study the effects of inhomogeneous conditions in a multicompartment geometry. In this case, the injected aerosol had to pass a chain-type arrangement of subcompartments during the transport from the central injection room to the dome compartment. The experiments clearly show the enhancement of the aerosol deposition by condensing steam (Fig. 2). Another important result from the tests was the observation that inhomogeneous condi-

tions can be introduced easily by suitable thermalhydraulic injection conditions, leading to atmospheric stratication. An international code benchmark exercise was conducted on the basis of DEMONA test B3 (Schock, 1987), with the following participants and codes; Table 2. The calculated aerosol concentrations are shown together with the experimental data in
Table 2 Participants and codes of the DEMONA B3 code benchmark exercise Participant ASTEN, Rome ENEL, Milano GRS, Koln KfK, Karlsruhe RNL, Ris SWEC, Boston JRC, Ispra SEAB, Nykoping SRD, Warrington UPM, Madrid Code NAUA Mod5 NAUA Mod5 FIPLOC-NAUA Mod5-M NAUA Mod5 NAUA Mod5 NAUA Mod4, enhanced (a) CORRAL-2/CORRADI (b) CONTAIN 1.04 MAAP-3 AEROSIM-M HAARM-DTN

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Table 1 DEMONA test matrix Experiment no. Performed Experimental condition Atmosphere Air Steam/air Aerosol material Max. conc. (g m3) Cont. geometry Single compartment Multi-compartment Remarks

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Steady-state Al B2 B3 B4 B5 B6 A7 A8 A9 October 1983 November 1984 November 1984 March 1985 May 1985 June 1985 November 1985 March 1986 May 1986 2.5 bar/20C

Steady-state 3 bar/115C 3 bar/115C 3 bar/115C 3 bar/115C 3 bar/115C

Transient Max. 3 bar Max. 3 bar Max. 3 bar

SnO2

Fe2O3 Ag Stratied atmosphere Homogenized atmosphere Homogenized atmosphere Homogenized atmosphere Homogenized atmosphere Stratied atmosphere 2 aerosol inject. Periods

No aerosols 12 8.4 6 12.4 Mixture, Mixture 7.0 3 4.5 1 x x x x x x x x

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Fig. 3. Calculated aerosol concentrations, NAUA versions. Symbols indicate measured data.

Figs. 3 and 4. For most calculations, the steam condensation on the aerosol particles was based on a volume condensation rate taken from a single-zone thermal hydraulic simulation using the COCMEL code. In Fig. 3, NAUA Mod5 results are shown from ASTEN, ENEL, KfK and RNL. The SWEC curve was calculated using an enhanced NAUA Mod4 version including the diffusiophoresis effect. The GRS curve was obtained from a multicompartment model using the coupled codes FIPLOC and NAUA Mod5-M; the

seven-zone model shows homogeneous atmospheric conditions during the aerosol deposition phase. The GRS model does not include steam condensation on the aerosols, while the others do so. From the comparison of the curves in Fig. 3, it can be concluded that model uncertainties (e.g. thermal hydraulic conditions, leakage rates, deposition models, user-specied parameters, etc.) are comparable to the effects of steam condensation on the aerosol; otherwise, the slope of the GRS curve should be much less than the slopes of the other curves.

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In Fig. 4, a variety of other codes results is shown. The irregular trends of several curves indicate nonphysical model behaviour. CONTAIN is a code that performs a fully-coupled solution of the thermal hydraulics and the aerosol dynamics, but the results are not much better than the other curves. It has to be pointed out that this was an open benchmark exercise, where the participants could tune their calculations to give a better approximation to the data. The lack of thermal hydraulics-

aerosol coupling and the necessity of manual parameter selection lead to a considerable spread in the results. At the time of the DEMONA B3 benchmark (1987), reliable predictions for reactor applications could hardly be expected, rather than some conservative estimates of ssion product leakage rates. Especially, multicompartment modeling of aerosols was only in its initial phase. The benchmark results are not detailed enough to validate individual submodels in the codes.

Fig. 4. Calculated aerosol concentrations, other codes. Symbols indicate measured data.

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Fig. 5. Measured and calculated pressure transients, CONTAIN participants.

3.2. VANAM
The VANAM experiments were conducted in the BMC in 1990 1992 to investigate aerosol behaviour in a multicompartment containment under realistic thermal hydraulic conditions (Kanzleiter et al., 1991). They differ from the DEMONA experiments in the following aspects: enhanced separation of subcompartments; more comprehensive instrumentation; thermalhydraulic transient oriented after scenario ND* of German Risk Study Phase B; and the use of insoluble and soluble aerosol material The experiments were conducted in two blocks. The rst block, tests M1 and M2, was executed to provide a rst set of data for analysis. After test M2, a 1 year interrupt was used to evaluate the results, to perform numerical simulations with the FIPLOC code, and to design the second block of experiments with some improvements in test geometry, operating procedure and instrumentation. The second block of tests was used intensively for code validation, especially including the International Standard Problem ISP 37 (Firnhaber et al., 1996). The geometry of the BMC is shown in Fig. 1, but for the VANAM tests the injection positions were modied. As compared to the DEMONA

geometry, separation of subcompartments is enhanced by closing the connections between the annulus and the inner rooms (R9.4R6 and R8) and in the inner cylinder (R3R1 and R1R2). Different ow recirculation loops are possible, and the establishment of ow circulation under elevated level injection (in R5) presents a challenge to simulation models and measurement. The thermalhydraulic instrumentation consists of several systems to measure the steam and air mass ow injected, some pressure gauges, a very large number of thermocouples for measuring atmosphere, sump and structure temperatures, two heat transfer measuring blocks, ten turbine ow meters to detect large-scale convection effects, eight capacitive humidity measuring systems, and three calorimeters to determine the droplet content in the atmosphere during periods of fog formation. The backbone of the aerosol instrumentation are eight lter stations installed inside the containment, each prepared to take 12 lter samples during a VANAM experiment. After the experiment the lter deposits can be evaluated by weighing and scanning electron microscopy to determine aerosol mass concentration and aerosol size distribution as a function of time and location. In addition, local aerosol concentration and possible fog formation (volume condensation) are

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K. Fischer, T. Kanzleiter / Nuclear Engineering and Design 191 (1999) 5367 Table 4 ISP 37 Benchmark participants and their codes Participant CIEMAT, Spain ECN, Netherlands Kurchatov Institute, Russia VUJE, Slovakia FZK, Germany CTN, Spain ENEA, Italy KAERI, Korea NUPEC, Japan Russian Academy of Sciences, Russia Sandia Nat. Lab., USA Studsvik, Sweden Russian Inst. Atom. Reactor, Russia GRS, Germany and IPSN, France IFE, Germany JRC, Italy Battelle, Germany University of Pisa, Italy ENEL, Italy IKE, Germany JAERI, Japan Code CONTAIN CONTAIN CONTAIN and MELCOR CONTAIN and MELCOR CONTAIN MELCOR MELCOR MELCOR MELCOR and MACRES MELCOR MELCOR, enhanced MELCOR MELCOR FIPLOC and RALOC FIPLOC FIPLOC GOTHIC (Thermal/Hydraulics only) FUMO (Thermal/Hydraulics only) ECART MOSAIC (Aerosol only) REMOVAL (Aerosol only)

continuously monitored by eight extinction photometers. During the second block of experiments, the following test procedure was applied; Table 3. Using this procedure, the following experiments were conducted: M2* using non-hygroscopic SnO2 aerosol M3 using hygroscopic NaOH aerosol M4 using a mixed aerosol of SnO2 and NaOH Experiment M3 was used as basis for the ISP 37. The results of this ISP will now be discussed briey; for more details, see Firnhaber et al. (1996). The benchmark participants and their codes were; Table 4. Like in the DEMONA B3 exercise, the ISP 37 was also conducted as an open benchmark with the experimental results published in advance. Most of the calculations used a mesh with 10 15 nodes. Only MOSAIC is based on a single-node approximation. RALOC calculates thermal hydraulics only, and MACRES is an aerosol only code. CONTAIN, MELCOR, FIPLOC and ECART are fully integrated codes for simultaneous calculation of thermal hydraulics and aerosol dynamics. The codes MACRES and REMOVAL also have multicompartment capability. Fig. 5 shows measured and calculated pressure transients. Deviations from the experimental data are mainly caused by errors in modeling the leakTable 3 Test procedure for second VANAM block Phase I II III IV V VI Duration (h) 15 1 5 0.5 2 5 Action Heat-up of test facility by steam injection First aerosol injection in upper room R5 Passive cool-down Second aerosol injection in R5 Mixing by steam injection to lower room R3 Steam injection to upper room R5

age of the facility, thermal outer boundary conditions, heat transfer to the walls, and simulation of mixed atmospheric conditions where the experiment shows a stratication. In fact, stratied conditions prevailed in the test during all phases except phase V, where mixing was introduced by steam injection to R3. Articial mixing shows up in a number of calculations where nodalization errors occurred, like the use of double ow paths with different elevation data. Most MELCOR simulations fail to predict the stratication in the inner rooms due to a too high time step applied (typically Dt 10 s instead of Dt 1 s). In Fig. 6, the measured and calculated aerosol concentrations in the dome subcompartment are shown. In phase III, the conditions are slightly superheated, such that the hygroscopic growth of the particles is of major importance with respect to the aerosol settling behaviour. In the CONTAIN calculations of VUJE and KI, the hygro-

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Fig. 6. Measured and calculated aerosol concentrations for (a) CONTAIN participants; (b) MELCOR participants; and (c) FIPLOC participants.

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scopic option was not activated. This model feature could explain the high concentration data of VUJE in phase III, but not the irregular curve of KI. In phase V, intense fog formation causes a rapid growth of all particles, and the hygroscopic effect is of minor importance. The high concentrations of the VUJE calculation in phases V and VI cannot be explained by the missing hygroscopic option. The extreme concentration decrease in phase V calculated by ECN is related to their use of a radiation heat transfer model option which leads to a too high steam condensation on the particles. CIEMAT calculated the proper thermal stratication between the dome and the lower room R3, but not the corresponding difference between high aerosol concentrations in the dome and low concentrations in R3 during phase III. The general impression from the CONTAIN calculations is that the balance of the individual submodels requires a high degree of user experience with the code. The present code documentation does not enable the majority of the benchmark participants to establish a consistent simulation of all major features observed in the experiment. The largest group of participants applied the MELCOR code. The deviations between calculated and measured aerosol concentrations indicated in Fig. 6 are mainly related to the missing option of aerosol hygroscopicity in MELCOR, and the inability to simulate the stratied atmospheric conditions. The calculation of SNL with an enhanced MELCOR version including the hygroscopic option does not show much improvement. The decay of the dome concentration under high fog formation, phase V, is mostly underpredicted. For the MELCOR group, similar (or even more severe) shortcomings in code documentation and user support can be recognized, as was the case for the CONTAIN group. More consistent results are found in the comparison between FIPLOC calculations and experimental aerosol data. Major differences by IFE during phase V and VI are related to an articial mixing introduced by a double ow path between dome R9.2 and annulus R9.3. The FIPLOC simulations show both stratied temperatures and aerosol concentrations in reasonable agreement

with the measurements. Apparently, the code documentation and the available options enable the user to sufciently control the model behaviour and to generate meaningful results. As compared to the DEMONA benchmark, the ISP 37 clearly shows that multi-compartment simulations are state-of-the-art, and local inhomogeneous distributions are of major relevance.

3.3. KAEVER
The KAEVER series of aerosol experiments were conducted during 19911996 by Battelle, Frankfurt (Po et al., 1997). The intention of the experiments was to investigate special effects of relevance to the aerosol deposition. The main focus was on the behaviour of soluble (CsI, CsOH), insoluble (Ag, SnO2) particles and aerosol mixtures (Ag/CsI, Ag/CsOH, CsI/CsOH, CsI/ CsOH/Ag) under various thermalhydraulic conditions in a well controlled vessel of 10 m3 volume. The test vessel was a horizontal steel cylinder of 2 m diameter and 2.5 m length, with access doors on both ends. Parts of the access doors were not isolated, while the major surfaces were equipped with isolation and controllable electric heating elements. Injection systems for steam, nitrogen and aerosols were provided, and the leakage rate was controlled by repeated tests. The thermal behaviour, effective heat capacities and heat losses to the environment were evaluated by heating tests, control of the external temperature distribution, and model simulations. Model calculations of the internal natural convection ow pattern indicated that well mixed conditions in the vessel were obtained within 12 min. The instrumentation is indicated in Fig. 7, covering pressure, atmospheric and structural surface temperature distribution, and relative humidity. An innovative technique was applied by using a spectral absorption photometer, which allows to determine in-situ and on-line fog droplet concentrations and size distributions. Conventional aerosol instrumentation was applied for redundant measurements of aerosol concentrations and size spectra:

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Filters (evaluated by weighing and electron microscopy); differential mobility particle sizer; aerodynamic particle sizer; transmission photometer; impactor. Aerosols were generated by evaporation from crucibles in induction-heating furnaces. A total of 33 main experiments were conducted, with a systematic variation of the following parameters:

relative humidity: low, high, saturated, fog formation; aerosol material: non-soluble, soluble, mixtures, fog. The major experimental results with respect to the deposition rate of the aerosols are as follows (see also Fig. 8): 1. Similar rates were observed for soluble and insoluble aerosols under highly superheated atmospheric conditions;

Fig. 7. Instrumentation of the KAEVER test facility.

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Fig. 8. Relative aerosol concentration decay rates during KAEVER experiments.

2. under weakly superheated conditions (90% r.h.), the highly soluble CsOH shows a signicantly enhanced deposition rate, while the moderately soluble CsI behaves like the insoluble Ag; 3. under supersaturated conditions with moderate fog formation, the deposition rate increases in correspondence to the hygroscopicity of the aerosol material; 4. under high fog formation, the deposition rates of soluble aerosols indicate a saturation behaviour; CsI and CsOH show similar deposition rates; 5. the behaviour of mixed aerosols is predominantly determined by its hygroscopic component; 6. chemical reactions between components of mixed aerosols can have an impact on the deposition rate. The data were used for validation of the FIPLOC aerosol models in an extensive way. The main results of the code simulation are as follows: 1. The code calculates the proper volume condensation rate and size distribution of droplets;

2. decay rates of insoluble and soluble material under superheated conditions are predicted properly; 3. also, decay rates under supersaturated conditions are simulated well, using shape factors of 1 for spherical particles; 4. decay rates of soluble particles under high fog formation are slightly overpredicted due to the assumption of equilibrium particle growth.

4. Conclusions The experience from the experimental investigations and the related code benchmarks leads to the following conclusions: (a) The early assumption of homogeneous conditions in the containment atmosphere is unrealistic and cannot give a conservative estimate for the radioactivity release; (b) Models and experimental data for inhomogeneous conditions are available. Models have been validated on the basis of the data; (c) Code validation studies show the high importance of userselected model features. More work is necessary to reduce this user effect when real plant tran-

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sients are predicted; (d) As indicated by the FIPLOC simulations for ISP 37, suitable code construction and documentation can result in a considerable reduction of user effects and improved results; (e) Experimental data and validated models are presently missing with respect to two important phenomena: (1) decay heat effects; and (2) chemical interactions of aerosol materials; (f) Spatial resolution and modelling concept of present lumped-parameter codes appear as an adequate basis for aerosol behaviour simulation and further development. No relevant applications of codes based on multidimensional CFD (computational uid dynamics) have been observed.

Acknowledgements The research projects discussed in the present paper were funded by the German Federal Ministry of Education, Science, Research and Technology, BMBF, through the GRS Research Management Division, Cologne. This continuous support is gratefully acknowledged by the authors.

References
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Bunz, H. et al., 1987. NAUA Mod5 und NAUA Mod5-M, Zwei Computerprogramme zur Berechnung des Aerosolverhaltens im Containmentsystem eines LWR nach einem Kernschmelzunfall. Report KfK 4278. Firnhaber, M. et al., 1996. International Standard Problem ISP37. VANAM M3 A Multi-Compartment Aerosol Depletion Test with Hygroscopic Aerosol Material. Report NEA/CSNI/R(96)26. Gelbard, F., 1991. MAEROS User Manual. Report NUREG/ CR-1391 Jahn, H. et al., 1986. Description of the Mod2/85 Versions of the RALOC/FIPLOC Family, Part 1: Code System. Report GRS-A-1315. Jokiniemi, J., 1990. Effect of selected binary and mixed solutions on steam condensation and aerosol behaviour in containment. Aerosol Sci. Technol. 12, 891 902. Kanzleiter, T., et al., 1991. The VANAM experiments M1 and M2 test results and multicompartment analysis. J. Aerosol Sci. 22, S697 S700. Liljenzin, J.-O., et al., 1990. Report from the MARVIKEN-V/ DEMONA/LACE Workshop. Proceedings of the Workshop on Aerosol Behaviour and Thermal Hydraulics in the Containment, CSNI Report No. 176. Murata, K.K. et al., 1989. Users Manual for CONTAIN 1.1: A Computer Code for Severe Nuclear Reactor Accident Containment Analysis. Report NUREG/CR-5026. Po, G. et al., 1997. Versuche zum Verhalten von Kernschmelzaerosolen im LWR-Containment-KAEVER. Report BF-R-67863, Battelle Ingenieurtechnik GmbH, Eschborn. Schock, W., 1987. Assessment of the outputs from the various computer codes used in the Member States to study the behaviour of aerosols in LWR containments in case of severe accidents. Report to the CEC under Study Contract ECI-1413-B7210-85-D. Summers, R.M. et al., 1994. MELCOR Computer Code Manual. Report NUREG/CR-6119. Weber, G. et al., 1996. Benutzerhandbuch fur FIPLOC 3.0. Report GRS-A-2417.