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Nuclear Fuel: Part 1: Metallic Fuel

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Nuclear Fuel: Part 1: Metallic Fuel ANL-00/24 ANL-00/24 Argonne National Laboratory REVIEW OF OXIDATION RATES OF DOE SPENT NUCLEAR FUEL: PART 1: METALLIC FUEL by BRUCE A. HILTON Argonne National Laboratory, Argonne, Illinois 60439 operated by the University of Chicago for the United States Department of Energy under Contract W-31-109-Eng-38 Argonne National Laboratory, with facilities in the states of Illinois and Idaho, is owned by the United States Government and operated by The University of Chicago under the provisions of a contract with the Department of Energy. DISCLAIMER 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 The University of Chicago, nor any of their employees or officers, 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 document authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof, Argonne National Laboratory, or The University of Chicago. Available electronically at http://www.doe.gov/bridge Available for a processing fee to U.S. Department of Energy and its contractors, in paper, from: U.S. Department of Energy Office of Scientific and Technical Information P.O. Box 62 Oak Ridge, TN 37831-0062 phone: (865) 576-8401 fax: (865) 576-5728 email: [email protected] ANL-00/24 ARGONNE NATIONAL LABORATORY P.O. Box 2528 Idaho Falls, Idaho 83403 Review of Oxidation Rates of DOE Spent Nuclear Fuel Part 1: Metallic Fuel by Bruce A. Hilton Nuclear Technology Division Argonne National Laboratory November 2000 i ii TABLE OF CONTENTS Page ACRONYMS.................................................................................................................................. x ABSTRACT................................................................................................................................... xi I. INTRODUCTION ..................................................................................................................1 A. Background....................................................................................................................2 1. Grouping...............................................................................................................2 2. Compositions and Fuel Types ..............................................................................2 B. Fundamentals of Oxidation and Corrosion....................................................................4 1. Thermodynamics..................................................................................................5 2. Kinetics and Reaction Processes ..........................................................................6 3. Temperature Dependence...................................................................................10 C. Measurement and Analysis Techniques ......................................................................12 1. Reaction Rate Measurements .............................................................................12 2. Reaction Product Characterization.....................................................................13 3. Unit Conversion Factors.....................................................................................14 4. Software..............................................................................................................15 II. OXIDATION RATES OF URANIUM METAL .................................................................15 A. Mechanisms of Uranium Metal Oxidation ..................................................................16 1. Uranium/Oxygen Reaction.................................................................................16 2. Uranium/Water Vapor Reaction.........................................................................17 3. Uranium/Water Reaction....................................................................................21 B. Kinetics of Uranium Metal Oxidation .........................................................................23 1. Uranium/Oxygen Reaction.................................................................................23 2. Uranium/Water Vapor Reaction.........................................................................29 3. Uranium/Water Reaction....................................................................................36 4. Summary ............................................................................................................39 C. Irradiation Effects on Uranium Metal Oxidation.........................................................40 D. Uranium-Hydride Effects on Uranium Metal Oxidation.............................................43 III. OXIDATION RATES OF URANIUM METAL ALLOYS.................................................45 A. Factors Affecting Uranium Alloy Oxidation...............................................................45 1. Microstructural Effects on Oxidation.................................................................45 2. Discontinuous Failure.........................................................................................47 B. Kinetics of Uranium-Molybdenum Oxidation ............................................................48 1. U-Mo/Water Vapor Reaction .............................................................................48 2. U-Mo/Water Reaction ........................................................................................49 C. Kinetics of Uranium-Niobium Oxidation....................................................................51 1. U-Nb/Water Reaction.........................................................................................51 D. Kinetics of Zirconium-Uranium Oxidation .................................................................53 1. Zr-U/Oxygen Reaction.......................................................................................54 2. Zr-U/Water Reaction..........................................................................................54 E. Irradiation Effects on Uranium Alloy Oxidation.........................................................55 F. Summary of Uranium Alloy Oxidation.......................................................................56 iii IV. OXIDATION RATES OF ALUMINUM-BASED DISPERSION FUELS.........................57 A. Oxidation Mechanisms of Aluminum-Based Dispersion Fuels ..................................58 1. Microstructural Effects on Oxidation.................................................................59 2. Oxidation Mechanism of Aluminum-Based Dispersion in Water .....................62 B. Kinetics of Aluminum Alloy Oxidation ......................................................................62 1. Al-Alloy/ Water Reaction ..................................................................................62 C. Kinetics of Aluminum Matrix-Uranium Aluminide Oxidation...................................64 1. Al-UAlx/Water Vapor Reaction..........................................................................64 2. Al-UAlx/Water Reaction.....................................................................................65 D. Kinetics of Aluminum Matrix-Uranium Oxide Oxidation ..........................................66 E. Kinetics of Aluminum Matrix-Uranium Silicide Oxidation........................................66 1. Al-UxSiy/Water Reaction ....................................................................................67 2. UxSiy/Oxygen Reaction.......................................................................................68 3. UxSiy/Water Reaction .........................................................................................69 F. Summary of Aluminum-Based Dispersion Fuel Oxidation ........................................70 V. CONCLUSIONS ..................................................................................................................71 VI. ACKNOWLEDGMENTS ....................................................................................................75 VII. REFERENCES .....................................................................................................................76 iv LIST OF FIGURES Figure 1. Schematic representation of metals oxidation: (a) adsorption of oxygen molecules, (b) dissociation of adsorbed oxygen molecule, and (c) continued growth by diffusion or migration of oxygen and metal ions through oxide. ...........4 Figure 2. Schematic illustration of the kinetic rate equations representing metal oxidation. .................................................................................................................7 Figure 3. Oxidation mechanisms represented by linear kinetics (a) surface reaction (b) parabolically growing oxide that periodically cracks and (c) weight gain versus time for (b)....................................................................................................9 Figure 4. Paralinear oxidation described by an inner, coherent layer that transforms to an outer, porous
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