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Demonstration of the TRUEX Process for Partitioning of Actinides from Actual ICPP Tank Waste ... PDF

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INEL-96/0353 September 1996 Idaho National Engineering Demonstration of the TRUEX Process Laboratory for Partitioning of Actinides from Actual ICPP Tank Waste Using Centrifugal Contactors in a Shielded Cell Facility J. D. Law K. N. Brewer R. S. Herbst T. A. Todd OF THIS DOCUMEtiT IS LOCK H E E D MARTIN^ INEL 96/0353 Demonstration of the TRUEX Process for Partitioning of Actinides from Actual ICPP Tank Waste Using Centrifugal Contactors in a Shielded Cell Facility J. D. Law K. N. Brewer R. S. Herbst T. A. Todd Published September 1996 Idaho National Engineering Laboratory Waste Management Technologies Lockheed Martin Idaho Technologies Company Idaho Falls, Idaho 83415 Prepared for the U.S. Department of Energy Assistant Secretary for Environmental Management Under DOE Idaho Operations Office Contract DE-AC07-94ID13223 DISCLAIMER Portions of this document may be illegible in electronic image products. Images are produced from the best available original document. , 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 any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or use- fulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any spe- cific commercial product, process, or service by trade name, trademark, manufac- turer, or otherwise does not necessarily constitute or imply its endorsement, recom- mendation, 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. ABSTRACT The TRUEX process is being evaluated at the Idaho Chemical Processing Plant (ICPP) for the separation of the actinides from acidic radioactive wastes stored at the ICPP. These efforts have culminated in a recent demonstration of the TRUEX process with actual tank waste. A continuous countercurrent flowsheet test was successfully completed at the ICPP using waste from tank WM-183. This demonstration was performed using 24 stages of 2-cm diameter centrifugal contactors installed in the shielded hot cell at the ICPP Remote Analytical Laboratory. The flowsheet tested consisted of eight extraction stages, five scrub stages, six strip stages, three solvent wash stages, and two acid rinse stages. It was determined that a centrifugal contactor stage in the scrub section was not operational during testing. As a result, the scrub feed (aqueous) solution followed the solvent into the strip section, effectively eliminating the scrub section in the flowsheet. An overall removal efficiency of 99.97% was obtained for the actinides. As a result, the activity of the actinides was reduced from 457 nCi/g in the feed to 0.12 nCi/g in the aqueous raffinate, which is well below the NRC Class A LLW requirement of 10 nCi/g for non-TRU waste. The 0.04 MHEDPA strip section back-extracted 99.9998% of the actinide activity from the TRUEX solvent. Removal efficiencies of >99.90%, 99.96%, 99.98%, >98.89%, 93.3%, and 89% were obtained for 241Am 238Pu, 5 239Pu, 23SU, 238U, and "Tc, respectively. Iron was partially extracted by the TRUEX solvent, resulting in 23% of the Fe exiting in the strip product. Mercury was also extracted by the TRUEX solvent (73%) and stripped from the solvent in the 0.25 MNa2CO wash section. Only 1.4% of the Hg exited with the high- 3 activity waste strip product. Data/results of this testing have been independently reviewed by personnel from Argonne National Laboratory. in ACKNOWLEDGEMENTS The authors would like to acknowledge the EM-50 Tanks Focus Area (TFA) for providing funding for this demonstration. They would also like to acknowledge C. P. McGinnis and the TFA Technical Review Group for their support of this program. The authors would like to thank George Vandegrift, Ralph Leonard, and Monica Regalbuto of ANL-East for their thorough technical review of the program and experimental results, and for participating in the demonstration. Many thanks to E. L. Wade, M. E. Davis, C. W. Lundholm, and G. D. Decoria for their assistance in installation and operation of the centrifugal contactors and T. G. Garn and R. D. Tillotson for their assistance with chemical makeup and sample preparations. Also, thanks to T. J. Tranter, D. Thomas, I. D. Goodwin, and B. J. Storms of the Radiochemical Analysis Group, R. W. Stone of the Spectrochemical Analysis Group, and the RAL Chemists and Analysts for the efficient, expedient sample analysis results. Without the work and dedication of these people, this test could not have succeeded. CONTENTS ABSTRACT iii ACKNOWLEDGEMENTS v INTRODUCTION 1 PURPOSE AND SCOPE 2 EQUIPMENT DESCRIPTION 3 METHODOLOGY/EXPERIMENTAL PROCEDURE 5 WM-183 Waste 5 TRUEX Solvent 6 Analytical 6 TRUEX Flowsheet Demonstration 7 RESULTS AND DISCUSSION 10 TRUEX Flowsheet Demonstration 10 Contactor Operation 10 Time to Reach Steady State ..10 Concentrations at Shutdown 12 Nitric Acid 15 Gross Alpha 15 Americium 15 Plutonium 16 Uranium 16 Technetium 16 Iron 17 Mercury 17 Comparison With Results Obtained Using SBW Simulant 17 CONCLUSIONS AND RECOMMENDATIONS 19 Conclusions 19 Recommendations 19 REFERENCES 20 Appendix A Experimental Data A-l vu TABLES Table 1. Description of the 2-cm centrifugal contactors 3 Table 2. WM-183 waste and average SBWtank compositions 5 Table 3. Flowrates and O/A ratios for TRUEX flowsheet testing 10 Table 4. Percentage of component in each of the effluent streams for TRUEX flowsheet testing 14 Table 5. Gross alpha, 24IAm, olPu, 239Pu, 23SU, and ™*U distribution coefficients for TRUEX flowsheet testing 14 Table 6. H+, Fe, and Hg distribution coefficients for TRUEX flowsheet testing 15 Table 7. Composition of simulated SBW 18 Table 8. Comparison of results obtained with simulant and actual waste 18 FIGURES Figure 1. 2-cm diameter centrifugal contactors installed in the RAL shielded cell 4 Figure 2. Flowsheet for TRUEX demonstration 8 Figure 3. Aqueous raffinate approach to steady state 11 Figure 4. Strip product approach to steady state 11 Figure 5. Actinide approach to steady state, strip product 12 Figure 6. TRUEX flowsheet test concentrations at shutdown 13 vm

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by contacting them twice with chlorinated cobalt dicarbollide at an O/A = 3/5. dicarbollide removes Cs and Sr, the primary beta emitters. J. A. Murphy, L. F. Pincock, and I. N. Christiansen, ICPP Radioactive Liquid and Calcine
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