ORNL/TM-2019/1459 Campaign 76—Production of 252Cf and the Recovery of Curium Feed Material at the Radiochemical Engineering Development Center Alan M. Krichinsky Dennis E. Benker Julie G. Ezold Jon R. Garrison Riley D. Hunley Roger J. Weaver December 2019 Approved for public release. Distribution is unlimited. 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-2019/1459 Isotopes and Fuel Cycle Technology Division CAMPAIGN 76—PRODUCTION OF 252CF AND THE RECOVERY OF CURIUM FEED MATERIAL AT THE RADIOCHEMICAL ENGINEERING DEVELOPMENT CENTER Alan M. Krichinsky Dennis E. Benker Julie G. Ezold Jon R. Garrison Riley D. Hunley Roger J. Weaver December 2019 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 LIST OF FIGURES .......................................................................................................................................v LIST OF TABLES.......................................................................................................................................vii ACRONYMS................................................................................................................................................ix 1. REDC FACILITY AND CAMPAIGN 76 PROCESSING OVERVIEW.............................................1 1.1 REDC FACILITY........................................................................................................................1 1.2 CALIFORNIUM CAMPAIGN—GENERAL OVERVIEW.......................................................2 1.3 CAMPAIGN 76—SUMMARY...................................................................................................4 1.4 CAMPAIGN 76—REPORT ORGANIZATION AND NOMENCLATURE.............................6 2. 76DS—ALUMINUM SHROUD AND TARGET DISSOLUTION.....................................................9 2.1 76DS-1—DISSOLUTION OF ALUMINUM COOLING SHROUDS (SCRAP) ......................9 2.2 76DS-2—DISSOLUTION OF TARGET....................................................................................9 3. 76CL—CLEANEX BATCH SOLVENT EXTRACTION FOR TRANSPLUTONIUM PURIFICATION..................................................................................................................................14 3.1 76CL-1—CLEANEX FEED ADJUSTMENT ..........................................................................14 3.2 76CL-1—CLEANEX EXTRACTION ......................................................................................15 3.3 76CL-1—CLEANEX SCRUBBING.........................................................................................15 3.4 76CL-1—CLEANEX STRIPPING ...........................................................................................16 4. 76CM—ACTINIDE AND LANTHANIDE SEPARATION BY LICL-BASED ANION EXCHANGE........................................................................................................................................20 4.1 76CM-1—LICL-BASED ANION EXCHANGE—1................................................................20 4.2 76CM-2—LICL ANION EXCHANGE—2 ..............................................................................24 4.3 76CM-3—LICL ANION EXCHANGE—3 ..............................................................................27 4.4 76CM-3(LIOH)—CONVERSION OF TRANSCURIUM ACTINIDES TO NITRATE FORM BY HYDROXIDE PRECIPITATION ..........................................................................30 5. 76CX—AHIB CATION EXCHANGE FOR TRANSCURIUM SEPARATION ..............................32 5.1 76CX-1—AHIB CATION EXCHANGE FOR TRANSCURIUM SEPARATION .................33 5.2 76CX-2—AHIB CATION EXHANGE FOR TRANSCURIUM SEPARATION....................36 6. 76BX—BERKELIUM PURIFICATION USING BATCH SOLVENT EXTRACTION............40 6.1 76BX-1—BERKELIUM PURIFICATION USING BATCH SOLVENT EXTRACTION.........................................................................................................................40 7. 76CF—CALIFORNIUM CAPSULE LOADINGS.............................................................................43 7.1 76CF-1—CALIFORNIUM LOADING INTO NUT PACKAGE D-101 ...............................43 7.2 76CF-2—CALIFORNIUM LOADING INTO NUT PACKAGE D-102 ...............................44 7.3 76CF-3—CALIFORNIUM LOADING INTO NUT PACKAGE D-103 ...............................44 8. 76CX-3—CATION EXCHANGE RECOVERY AND PURIFICATION OF LOADING- RESISTIVE CALIFORNIUM.............................................................................................................46 8.1 76CX-3—CATION EXCHANGE RECOVERY AND PURIFICATION OF LOADING-RESISTIVE CALIFORNIUM ...............................................................................46 9. 76CF-4—CAPSULE LOADING WITH LOADING-RESISTIVE CALIFORNIUM .......................48 9.1 76CF-4—CALIFORIUM LOADING INTO NUT PACKAGE D-104...................................48 10. 76OH—HYDOROXIDE PRECIPITATION FOR LICL REMOVAL FROM TRANSCURIUM ACTINIDES ..........................................................................................................49 10.1 76OH-1 HYDROXIDE PRECIPICATION FOR LICL REMOVAL FROM TRANSCURIUM ACTINIDES ................................................................................................49 10.2 76OH-2 HYDROXIDE PRECIPICATION FOR LICL REMOVAL FROM TRANSCURIUM ACTINIDES ................................................................................................50 11. CAMPAIGN 76 REWORK.................................................................................................................52 11.1 CY15F115CL-1 CLEANEX REWORK ...................................................................................52 iii 11.2 CY15T23CL-1A CLEANEX REWORK ..................................................................................53 11.3 CY15T23CL-1B CLEANEX REWORK...................................................................................53 12. 76OX AMERICIUM/CURIUM OXALIC ACID PRECIPITATION AND PURIFICATION (OX) .....................................................................................................................................................55 12.1 76OX-1 AMERICIUM/CURIUM OXALIC ACID PRECIPITATION AND PURIFICATION........................................................................................................................55 12.2 76OX-2 AMERICIUM/CURIUM OXALIC ACID PRECIPITATION AND PURIFICATION........................................................................................................................56 12.3 76OX-3 AMERICIUM/CURIUM OXALIC ACID PRECIPITATION AND PURIFICATION........................................................................................................................57 12.4 76OX-4 AMERICIUM/CURIUM OXALIC ACID PRECIPITATION AND PURIFICATION........................................................................................................................57 13. CAMPAIGN 76 SUMMARY .............................................................................................................60 REFERENCES.............................................................................................................................................63 APPENDIX A. CAMPAIGN 76 PLAN....................................................................................................A-1 APPENDIX B. LIST OF SAMPLE CODES.............................................................................................B-1 iv LIST OF FIGURES Figure 1. Cross-sectional view of the hot cell bank.......................................................................................2 Figure 2. Top-level flow sheet of C76. ..........................................................................................................5 Figure 3. Target and rework material dissolution