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Potential Effects of Gallium on Cladding Materials

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Potential Effects of Gallium on Cladding Materials ORNL/TM-13504 OAK RIDGE NATIONAL LABORATORY Potential Effects of Gallium on LOCKHEED MARTIN Cladding Materials Dane F. Wilson Edward C. Beahm Theodore M. Besmann Jackson H. DeVan James R. DiStefano Uri Gat Sherrell R. Greene Phillip L. Rittenhouse Brian A. Worley MANAGED AND OPERATED BY LOCKHEEDMARTIN ENERGY RESEARCHCORPORATION FOR THE UNITED STATES DEPARTMENT OF ENERGY ORNL-27 (3-96) This report has been reproduced directly from the best available copy. Available to DOE and DOE contractors from the Office of Scientific and Technical Information, P. O. Box 62, Oak Ridge, TN 37831; prices available from (423) 576-8401. Available to the public from the National Technical Information Service, U.S. Department of Commerce, 5285 Port Royal Rd., Springfield, VA 22161. 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, appratus, 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-13504 Metals and Ceramics Division Potential Effects of Gallium on Cladding Materials Dane F. Wilson Edward C. Beahm Theodore M. Besmann Jackson H. DeVan James R. DiStefano Uri Gat Sherrell R. Greene Philip L. Rittenhouse Brian A. Worley Date Published: October 1997 NOTICE: This document contains information of a preliminary nature. It is subject to revision or correction and therefore does not represent a final report. Prepared for the U.S, Department of Energy Office of Fissile Materials Disposition GA 01 02 01 4 Prepared by the OAK RIDGE NATIONAL LABORATORY Oak Ridge, Tennessee 37831-6285 managed by LOCKHEED MARTIN ENERGY RESEARCH for the U.S. DEPARTMENT OF ENERGY under contract DE-AC05-96OR22464 CONTENTS LIST OF TABLES ............................................................ iv ACRONYMS ................................................................. v EXECUTIVE SUMMARY ..................................................... vi 1. INTRODUCTION .......................................................... 1 2. GALLIUM IN WG MOX FUEL ............................................... 2 2.1 AS-FABRICATED WG MOX FUEL .................................... 2 2.2 CHEMISTRY ...................................................... 2 2.2.1 Agglomerates ............................................. 2 2.2.1.1 Oxidation potential ................................... 2 2.2.2 Bulk Fuel Chemistry ......................................... 9 2.2.2.1 Oxide formation ..................................... 9 2.2.3 Reactions with Fission Products ............................... 10 2.3 GALLIUM TRANSPORT MECHANISMS WITHIN FUEL ................. 10 2.3.1 Gas Phase Transport ......................................... 10 2.3.2 Solid-State Transport ........................................ 12 3. CLAD PERFORMANCE AND DEGRADATION MECHANISMS .................. 15 3.1 INTRODUCTION ................................................. 15 3.2 FUEL-SIDE CORROSION ........................................... 17 3.2.1 Environment/Burnup ........................................ 17 3.2.2 Material Variables .......................................... 18 3.2.3 Pellet Clad Interaction ....................................... 19 3.2.4 Mechanisms of Gallium Embrittlement ......................... 19 3.3. WATERSIDE CORROSION ......................................... 21 4. GALLIUM AND FUEL PERFORMANCE: CONCLUSIONS AND RECOMMENDATIONS ................................................ 23 REFERENCES ............................................................... 26 APPENDIX PHYSICAL, CHEMICAL AND NUCLEAR CHARACTERISTICS OF GALLIUM AND GALLIUM OXIDES ..................................................A-1 A.1 ELEMENTAL GALLIUM ..........................................A-1 A.1.1 PHYSICAL CHARACTERISTICS ...........................A-1 A.1.2 CHEMICAL CHARACTERISTICS ..........................A-2 A.1.3 NUCLEAR CHARACTERISTICS OF GALLIUM ...............A-3 A.2 GALLIUM OXIDES ...............................................A-5 A.3 IMPURITIES ....................................................A-5 A.3.1 HALOGEN IMPURITIES ..................................A-5 A.3.2 CHALCOGENIDE IMPURITIES ............................A-6 A.3.3 REACTIONS WITH GROUP V ELEMENTS ...................A-6 A.4 REFERENCES ...................................................A-7 iii LIST OF TABLES Table 1. Fission product concentrations computed for a burnup of 52.5 MWd/kg and their oxidation state assuming gallium is present as the oxide in as-fabricated fuel ................ 6 Table 2. Fission product concentrations computed for a burnup of 52.5 MWd/kg and their oxidation state assuming gallium is present unoxidized in as-fabricated fuel ................. 7 Table 3. Thermodynamic values at 1000 K for the gallium-oxygen system ................ 11 Table A.1. Physical properties of gallium ........................................A-1 Table A.2. Gallium compounds with zirconium or plutonium .........................A-2 Table A.3. Chemical properties of gallium .......................................A-3 iv ACRONYMS BWR boiling-water reactor HE hydrogen embrittlement ISCC intergranular stress corrosion cracking LANL Los Alamos National Laboratory LME liquid metal embrittlement LWR light-water reactor MOX mixed oxide O/M oxygen-to-metal PCI pellet-clad interaction PWR pressurized-water reactor R&D research and development SCC stress corrosion cracking SMIE solid metal-induced embrittlement WG weapons grade v EXECUTIVE SUMMARY The Department of Energy has announced that the United States will pursue a dual-track approach to the disposition of plutonium arising from the dismantling of nuclear weapons. The dual-track disposition approach involves both immobilization and reactor-based mixed oxide (MOX) fuel technologies. The use of the MOX fuel option requires the assessment of the potential impact of gallium (on the order of 10 ppm), not present in conventional MOX fuel, on cladding material performance. This paper identifies and examines issues concerning the incorporation of gallium in weapons-derived plutonium in light water reactor (LWR) MOX fuels. Particular attention is given to the more likely effects of the gallium on the behavior of the cladding material. The chemistry of weapons-grade (WG) MOX, including possible consequences of gallium within plutonium agglomerates, was assessed. Based on the calculated oxidation potentials of MOX fuel, the effect that gallium may have on reactions involving fission products and possible impact on cladding performance were postulated. Gallium transport mechanisms are discussed. With an understanding of oxidation potentials and assumptions of mechanisms for gallium transport, possible effects of gallium on corrosion of cladding were evaluated. Potential and unresolved issues and suggested research and development (R&D) required to provide missing information are presented. This analysis concludes that without control of the stoichiometry of the MOX fuel it is possible for the gallium to be present as either elemental gallium or gallium sesquioxide (Ga 2O3) in the as-fabricated fuel. To keep gallium as a metal oxide in the as-fabricated fuel, the fuel oxygen-to-metal ratio (O/M) should be at least equal to 2. During burnup, in an isolated plutonia aggregate the fission products molybdenum, technetium, cadmium, tin, antimony, tellurium, and some ruthenium are computed to be present as oxides. At temperatures approaching >1200 K, the vapor pressure of gaseous gallium oxide 4 5 (Ga2O) will be of the order of 10 to 10 Pa. Within the fuel rod, the oxide species may vaporize in significant quantities in the hotter regions and transport to the cooler clad surfaces, where it would condense. Should this mode of mass transfer be particularly effective, reduction of the Ga2O3 by the zirconium in the clad could have detrimental effects on clad performance. However, significant burnup could serve to reduce this mode of mass transport. General corrosion of the cladding with gallium or gallium oxide is not a concern. General corrosion is mass limited, and the mass of gallium present in the fuel volume is low relative to the clad volume. However, localized corrosion (grain boundary penetration) and vi liquid-metal embrittlement by gallium are possible compatibility issues that need further investigation. The possibility that gallium will influence water (aqueous) corrosion is considered remote. vii 1. INTRODUCTION The Department of Energy announced in January 1997 that the United States will pursue a dual-track surplus plutonium disposition approach in which both immobilization and reactor- based mixed oxide (MOX) fuel technologies will be employed. Currently, more than a dozen commercial light-water reactors (LWRs) in Europe use recycled plutonium in MOX fuel assemblies. More than 300,000 LWR MOX fuel rods have been irradiated during the past decade. The performance of this commercial
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