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Off-Gas Performance and the Fission Product Mechanistic Source Term ORNL/TM-2018/958 Thermochemical and Transport Properties Important to Molten Salt Reactor Operation: Off-Gas Performance and the Fission Product Mechanistic Source Term Joanna McFarlane Charles F. Weber M. Scott Greenwood Approved for public release. A. Lou Qualls Distribution is unlimited. August 2018 DOCUMENT AVAILABILITY Reports produced after January 1, 1996, are generally available free via US Department of Energy (DOE) SciTech Connect. Website www.osti.gov Reports produced before January 1, 1996, may be purchased by members of the public from the following source: National Technical Information Service 5285 Port Royal Road Springfield, VA 22161 Telephone 703-605-6000 (1-800-553-6847) TDD 703-487-4639 Fax 703-605-6900 E-mail [email protected] Website http://classic.ntis.gov/ Reports are available to DOE employees, DOE contractors, Energy Technology Data Exchange representatives, and International Nuclear Information System representatives from the following source: Office of Scientific and Technical Information PO Box 62 Oak Ridge, TN 37831 Telephone 865-576-8401 Fax 865-576-5728 E-mail [email protected] Website http://www.osti.gov/contact.html This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. ORNL/TM-2018/958 Nuclear Security and Isotope Technology Division THERMOCHEMICAL AND TRANSPORT PROPERTIES IMPORTANT TO MOLTEN SALT REACTOR OPERATION: OFF-GAS PERFORMANCE AND THE FISSION PRODUCT MECHANISTIC SOURCE TERM Joanna McFarlane Charles F. Weber M. Scott Greenwood A. Lou Qualls August 2018 Prepared by OAK RIDGE NATIONAL LABORATORY Oak Ridge, TN 37831-6283 managed by UT-BATTELLE, LLC for the US DEPARTMENT OF ENERGY under contract DE-AC05-00OR22725 CONTENTS page ABSTRACT......................................................................................................................................4 1. INTRODUCTION...................................................................................................................................4 1.1. MSRs CONSIDERED AS TEST CASES ........................................................................................4 1.1.1.Impurities in Clean Salt ...........................................................................................................4 1.1.2.Fission Product Reservoirs under Normal Operation..............................................................5 1.1.3.Fission Product Inventory versus Burnup................................................................................6 1.1.4.High Dose Locations Outside the Core Coming from Delayed Neutrons...............................7 2. FISSION PRODUCT, ACTIVATION PRODUCT, AND REACTOR MATERIALS THERMOCHEMISTRY AND REACTION RATES.............................................................................8 2.1. SALT SOLUBLE FISSION PRODUCTS........................................................................................8 2.2. VOLATILE FISSION PRODUCTS AND DAUGHTERS..............................................................8 2.3. PRECIPITATES ...............................................................................................................................8 2.4. CORROSION OF METAL PIPING.................................................................................................9 2.5. RADIOLYSIS...................................................................................................................................9 2.6. OFF-EUTECTIC DRIFT ..................................................................................................................9 3. TRANSPORT PROPERTIES NEEDED TO DESCRIBE FISSION PRODUCT INVENTORY UNDER NORMAL OPERATING CONDITIONS..............................................................................11 3.1. HEAT TRANSFER IN SALT ........................................................................................................11 3.2. DIFFUSION OF FISSION PRODUCTS AND MINOR CHEMICAL SPECIES THROUGH SALT ............................................................................................................................................11 3.3. LOSS OF FISSION PRODUCTS TO THE HEAD SPACE ..........................................................11 3.4. PRECIPITATION OF SOLID FISSION PRODUCTS IN COOLER AREAS OF THE PHTS 3.5. GRAPHITE DEGRADATION.......................................................................................................12 3.6. AEROSOL FORMATION FROM MECHANICAL BREAKUP OF THE SALT........................12 3.7. REACTIVITY FEEDBACK ..........................................................................................................12 3.8. HEADSPACE GAS SPARGING AND OFF-GAS SYSTEM.......................................................12 4. ACCIDENT SCENARIOS POTENTIALLY ALLOWING FISSION PRODUCT RELEASE OR CONTAMINATION OF INTERNAL SYSTEMS ...............................................................................14 4.1. SCENARIOS LEADING TO BREECH IN PHTS ........................................................................14 4.1.1.Salt Leak ................................................................................................................................14 4.1.2.Crack in Headspace ...............................................................................................................14 4.1.3.Failure of heat exchanger.......................................................................................................14 4.2. FAILURE OF CHEMISTRY CONTROL......................................................................................15 4.2.1.Corrosion ...............................................................................................................................15 4.2.2.Failure of On-line Salt Processing.........................................................................................15 4.2.3.Failure of Off-Gas Removal System .....................................................................................15 4.3. SCENARIOS LEADING TO FLOW IRREGULARITIES ...........................................................15 4.3.1.Heat Exchanger Clogging......................................................................................................15 4.3.2.System and Component Malfunctions...................................................................................15 iii 5. SAFEGUARDS.....................................................................................................................................16 5.1. Assess the Need ..............................................................................................................................17 5.2. Methods for Monitoring Inventories...............................................................................................17 5.3. Securing the PHTS..........................................................................................................................17 5.4. Securing On- or Off-Line Salt Processing ......................................................................................17 5.5. Protection of Nuclear Waste ...........................................................................................................17 6. RECOMMENDATIONS ......................................................................................................................18 7. REFERENCES ......................................................................................................................................20 TABLES Page Table 1. Impurity Specifications for MSRE ..................................................................................................5 Table 2. Elements Generated from Operation of Selected MSRs..................................................................6 iv ABSTRACT The source term used in reactor performance and safety analysis requires understanding the chemical speciation and transport behavior of fission and activation products in the primary heat transport system (PHTS) and containment. As a starting condition, the transport models will use the isotopic compositions determined through ORIGEN (Bell 1973) calculations and thermochemistry that describes the speciation of the fuel, the salt, activation products and fission products. However, as changes in phase will be under non-equilibrium conditions, the source terms will also need models for the transport behavior of key compounds in the PHTS under various scenarios: normal operation with and without an off-gas system, maintenance, off-normal events, and severe reactor accidents. This document highlights those mechanistic behaviors for which models are needed. Simulations of reactor behavior require these models to be developed for molten salt reactors (MSRs), especially
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