ORNL/TM-2019/1283 Separation and Purification of Berkelium-249 and Einsteinium-254 R. A. Boll T. A. Dyer J. G. Ezold C. E. Phelps K. M. Phillips C. E. Porter J. L. Rayburn F. D. Riley N. J. Sims S. M. Van Cleve January 2020 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. 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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-2019/1283 Isotope and Fuel Cycle Technology Division Separation and Purification of Berkelium-249 and Einsteinium-254 Authors: R. A. Boll T. A. Dyer J. G. Ezold C. E. Phelps K. M. Phillips C. E. Porter J. L. Rayburn F. D. Riley N. J. Sims S. M. Van Cleve Date Published: January 2020 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 CONTENTS .................................................................................................................................................iii LIST OF FIGURES ......................................................................................................................................iii LIST OF TABLES........................................................................................................................................iii ACRONYMS................................................................................................................................................iii EXECUTIVE SUMMARY............................................................................................................................1 1. INTRODUCTION .................................................................................................................................2 1.1 BERKELIUM ..............................................................................................................................2 1.2 EINSTEINIUM............................................................................................................................2 2. EXPERIMENTAL PROCEDURES......................................................................................................3 2.1 OVERVIEW OF 249Bk FINAL PURIFICATION PROCEDURES ............................................3 2.1.1 Organic Solvent Scrubbing with Trichloroethylene (TCE) ............................................3 2.1.2 Volume Reduction and Cation-Exchange Feed Preparation...........................................4 2.1.3 Initial Cation-Exchange Cleanup Column ......................................................................5 2.1.4 AHIB Cation-Exchange Column ....................................................................................7 2.1.5 Final Cation-Exchange Cleanup Column .......................................................................9 2.2. OVERVIEW OF 254Es FINAL PURIFICATION PROCEDURES...........................................12 2.2.1. Initial Cation-Exchange Concentrator Column ............................................................12 2.2.2. AHIB Cation-Exchange Column ..................................................................................13 2.2.3. Final Cation-Exchange Cleanup Column .....................................................................15 3. PRODUCTION CAMPAIGNS ...........................................................................................................16 3.1. PRODUCTION CAMPAIGN 74...............................................................................................16 3.2. PRODUCTION CAMPAIGN 75...............................................................................................21 3.3. PRODUCTION CAMPAIGN 76...............................................................................................25 3.4. PRODUCTION CAMPAIGN 77...............................................................................................30 3.4.1. 249Bk Recovery..............................................................................................................30 3.4.2. 254Es Recovery ..............................................................................................................35 3.4.3. Attempted 257Fm Recovery ...........................................................................................42 4. INSTRUMENTATION .......................................................................................................................43 5. CONCLUSION....................................................................................................................................44 6. REFERENCES ....................................................................................................................................45 7. ACKNOWLEDGMENTS ...................................................................................................................46 iii LIST OF FIGURES Figure 1. Organic and aqueous layers in separatory funnel during TCE scrubbing. ...................................4 Figure 2. Condensation and reflux condenser unit with heating mantle......................................................4 249 Figure 3. Boiling flask with NO2 fumes and Bk solution. .......................................................................5 Figure 4. Initial cation-exchange cleanup column with 150 mL reservoir, showing elution into centrifuge tubes. ...........................................................................................................................5 Figure 5. Initial cleanup micro-glass cation-exchange column with 150 mL reservoir...............................6 Figure 6. The 249Bk product with “Bk green” color in centrifuge tube, before and after volume reduction.......................................................................................................................................7 Figure 7. Micro-glass jacketed AHIB cation-exchange column..................................................................8 Figure 8. AHIB column loaded with 249Bk solution, showing movement of green band............................9 Figure 9. Final cleanup micro-glass cation-exchange column...................................................................11 Figure 10. Final cation-exchange cleanup column with 249Bk solution loaded onto resin. .........................12 Figure 11. Initial cation-exchange concentrator column with 254Es product in a centrifuge tube after a column run. .....................................................................................................................13 Figure 12. AHIB column loaded with 254Es solution and the centrifuge containing the product. ...............14 iv LIST OF TABLES Table 1. Summary of purified 249Bk and 254Es harvested in Cf Campaigns 74 and 77................................1 Table 2. Feed material for C74 ..................................................................................................................16 Table 3. Dose rates and volumes of centrifuge tubes 1–8 from AHIB column separation .......................17 Table 4. Mass of 249Bk, 249Cf, and 252Cf in centrifuge tubes 1–8 ...............................................................20 Table 5. Analysis of 249Bk solution after final cleanup procedures ...........................................................20 Table 6. Dose rates and volumes of quartz cones sent to customers in Dimitrovgrad, Russia..................21 Table 7. Feed material for C75 ..................................................................................................................21 Table 8. Dose rates and volume of centrifuge tubes 1 and 2 after volume reduction................................22 Table 9. Dose rates and volumes of centrifuge tubes 3–6 after initial cleanup column ............................22 Table 10. Dose rates and volumes of centrifuge tubes 7–20 from AHIB column separation .....................23 Table 11. Mass of 249Bk, 249Cf,