Strontium-90 Heat Sources
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OAK RIDGE NATIONAL LABORATORY LIBRARIES 11111 11 111111 11 1111 111111 11 11 11 1111 111 11111 1111 11 111 111 1111 1 ORNl-IIC-36 ~. I CENTRAL '-- .::.ARCH LIBRARY DOCUMiNT COLLECTION STRON,TIUM-90 HEAT SOURCES Compiled and Edited by Robe rta Sho r Robert H. lafferty, Jr. P. S. Baker A strontium-90 powered light buoy ISOTOPES INFORMATION CENTER This report was prepared as an account of work sponsored by the United o States Government. Neither the United States nor the United States Atomic Energy Commission, nor any of their employees, nor any of their contractors, subcontractors, or 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. I I l ORNL-IIC-36 Contract No. W-7405-eng-26 • ISOTOPES INFORMATION CENTER STRONTIUM-gO HEAT SOURCES Compiled and Edited by Roberta Shor, Robert H. Lafferty, Jr., and P. S. Baker MAY 1971 OAK RIDGE NATIONAL LABORATORY Oak Ridge, Tennessee operated by UNION CARBIDE CORPORATION for the U. S. ATOMIC ENERGY COMMISSION .. .. FOREWORD This report deals primarily with the large-scale production operations carried out from 1958 to July 1967 by Oak Ridge National Laboratory, the Hanford Works, and the Martin Company for the preparation of strontium-90 heat sources. Some work done between 1948 and 1958 is summarized very briefly to provide a background for these operations. Also-a few later developments (from July 1967 to May 1970) have been included where possible. In writing this report, the editors have compiled summaries from experienced workers in the various phases of strontium fuel formation. We wish to acknowledge the original authors here. C. L. Ottinger wrote sections describing the Fission Products Development Laboratory building and facilities, the preparation of SrTi03 and SrO, the 85 Kr leak test of welded capsules, and the technique of cold-press and sinter formation of SrTi03 pellets. D. E. Horner reviewed the strontium separation processes carried out at Oak Ridge National Laboratory and at the Hanford Works. The numerous original authors in Horner's review article are referred to in Chapter 2. R. D. Seagren made many helpful suggestions about the section on transport of radioactive strontium and S. A. Reynolds summarized noncalorimetric analytical procedures. The calorimetric procedures are the work of J. C. Posey, T. A. Butler, P. S. Baker, and W. D. Box. R. E. McHenry contributed the major portion of the chapter on fuel fabrication including the development of the hot-press procedure. R. G. Donnelly wrote the section about capsule welding and E. E. Ketchen reported the measurement of thermal conductivity. Summaries from E. E. Pierce and E. Lamb describe the source examination. The properties of strontium fuel forms were compiled by S. J. Rimshaw and E. E. Ketchen. We thank the editors of Chemical Engineering Progress Symposium Series published by the American Institute of Chemical Engineers for permission to publish the material in Appendixes F and G. We are also indebted to A. F. Rupp and J. H. Gillette of Oak Ridge National Laboratory; R. L. Moore and H. H. Van Tuyl of Battelle-Northwest; and W. G. Ruehle of Aerojet-General Corporation for reviewing sections of the report and giving us their helpful criticism. iii GLOSSARY OF TERMS AGN Formerly Aerojet General Nucleonics Co.; now Aerojet Nuclear Systems Co. BAMBP 4-sec-bu tyl-2( Q-me thylbenzyl) phenol BNWL Battelle Northwest Laboratories Darex; Purex; Redox Solvent extraction processes for recovery of U and Pu from spent reactor fuels Decalso Inorganic ion exchange resin DOT Department of Transportation DOWEX SOW X 12 Organic ion exchange resin DTPA diethylenetriaminepentaac~~ic acid D2EHPA di(2-ethylhexyl)phosphoric acid EDTA ethylenediaminetetraacetic acid FPDL Fission Products Development Laboratory FTW formaldehyde treated waste Hanford or HAPO Hanford Atomic Products Operation, General Electric Co. (before 1965) HAPO lA, HAPO II Shipping casks HDEHP = D2EHPA di(2-ethylhexyl)phosphoric acid HEDTA (N-hydroxyethyl)ethylenediaminetriacetic acid kCi Kilocurie LCG Low Cost Generator (Martin Marietta Co. Nuclear Division) Martin Martin Marietta Co. Nuclear Division MeV Million electron volts Mitsubishi Mitsubishi Atomic Power Industries, Inc., Omiya, Japan MPC Maximum permissible concentration NaD2EHP sodium di(2-ethylhexyl)phosphate NasDTPA diethylenetriaminepentasodium acetate NUMEC Nuclear Materials and Equipment Corp., Apollo, Pa. lWW aqueous waste from solvent extraction uranium-plutonium recovery process that contains fission products ORNL Oak Ridge National Laboratory PAW Purex low-acid waste RCA Radio Corporation of America RIPPLE Radioisotope Powered Prolonged Life Equipment RTG Radioisotopic Thermoelectric Generator Sentinel Isotopes Inc. radioisotope thermoelectric generator SNAP Systems for Nuclear Auxiliary Power STW sugar treated waste TBP tributyl phosphate TIG Tungsten inert gas (welding method) TRACS Thermoelectric Radioisotope Conversion System TZM Refractory alloy; 99+% Mo, 0.5% Ti, 0.1 % Zr UKAEA United Kingdom Atomic Energy Authority URIPS Underwater Radioisotope Power Source W Watt v CONTENTS Foreword iii Glossary of Terms ........................................................................ v Abstract .......................................................................... : .... 1. Introduction ......................................................................... Selection of 90 Sr as Heat Source. 2 Operation of Radioisotope-Powered Electrical Generators ....................................... 2 2. Separation Processes ...... 9 Purity Requirements . .. 10 Precipitation Processes .................................................................. 11 Ion Exchange Processes. .. 12 Solvent-Extraction Processes. .. 12 3. Transportation and Building Facilities. .. 19 Shipment of Radioactive Material. .. 19 Fission Products Development Laboratory ... .. 22 4. Preparation of Strontium Titanate ......................................................... 27 Present Procedures for Compound Preparation . ... .. 27 Other Methods of Preparing SrTi03 ...•......•..........•....•......••...•.•.......•....... 30 Analytical Methods . .. 30 5. Fabrication of Fuels .................................................................... 35 Cold-Pressing and Sintering . .. 35 Hot Pressing .......................................................................... 39 Melt-Casting .......................................................................... 47 6. Source Encapsulation and Testing. ... ... .. 49 Welding of 90 Sr Containers. .. 49 Leak Testing ....................... ~ . .. 53 Heat Transfer and Thermal Conductivity .................................................... 59 7. Examination of Used Sources .. .. 63 RCA Test Source. .. 63 SrO Sources. .. 63 SNAP-7A Generator .................................................................... 66 8. Properties of Strontium Fuel Forms. .. .. .. .. .. 75 Explanation of Tables . .. 75 Composition ..... .. 75 Radiation ............................................................................ 75 Specific Power. .. 86 Physical and Chemical Properties .......................................................... 87 Thermophysical Properties ............................................................... 88 Compatibility with Containment Materials . .. 91 vii viii Appendix A ............................................................................. 97 Appendix B ............................................................................. ·99 Appendix C 101 Appendix D •••••••••••••••••••••••••••••••••••••••••••••••••••••••••••••••••••••• 0· •••••• 105 Appendix E 109 Appendix F III Appendix G 115 Appendix H ............................................................................. 123 Appendix I . .. 127 Appendix J . .. 131 Strontium -90 Heat Sources Compiled and Edited by Roberta Shor, Robert H. Lafferty, Jr., and P. S. Baker Abstract Strontium-90 heat source production is described. This includes purification, transportation, preparation of fuel forms, analytical methods, densification, encapsulation, source testing, and examination of used sources. Details of source preparation, encapsulation, and testing are given. 1. INTRODUCTION Compact electrical generators powered by heat from The report deals mainly with the large-scale produc radioisotopes have been under development in the tion operations from 1958 to July 1967 but also United States since the early 1950's for space, marine, summarizes very briefly work done from 1948 to 1958. and terrestrial uses. Essentially all the generators devel Most of the material deals with work that was previ oped for marine and terrestrial uses have been powered ously unreported or was described in reports having by 90 Sr. This report summarizes the development work liinited distribution. In the interest of continuity and done by Oak Ridge National Laboratory (ORNL) , coherence; however, certain portions are included Hanford Atomic Products Operation, * and Martin which have been adequately reported elsewhere: for Company, Nuclear Division, which led to the produc example, shipping, some aspects of the separation of tion of 90 Sr heat sources for use in the generators. fission products, and physical properties of the fuel Although the functions of the three contractors forms. The development, present practices,