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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report 6 Electrometallurgical Technology Demonstration Project Success Criteria INTRODUCTION The EBR-II Spent Nuclear Fuel Treatment Demonstration Project began in June 1996 and ended in June 1999. During the testing program, 100 EBR-II driver (core) fuel assemblies and up to 25 EBR-II blanket assemblies were to be processed. Waste form samples were to be prepared and tested. Sufficient data for evaluating the safety, environmental impact, and economics of the technology were to be generated. The committee, throughout the three phases of its study, recommended that ANL adopt criteria to evaluate the success of its demonstration project.1 The committee first proposed such criteria in its second report, recommending four separate criteria as accomplishments against which to evaluate the success of the demonstration project:2 Demonstration of batch operation of an electrorefiner and a cathode processor of approximately 200 kg/day of radioactive EBR-II spent fuel without failure for about 30 days. Quantification (for both composition and mass) of recycle, waste, and product streams that demonstrate projected material balance with no significant deviations. Demonstration of an overall dependable and predictable process, considering uptime, repair and maintenance, and operability of linked process steps. Demonstration that releases of radioactivity remain at or below those levels anticipated and specified in equipment design and operating plans. Exposure of operating personnel to radiation must be minimal and must in all cases remain below limits set by the U.S. Nuclear Regulatory Commission. In phase two of its study, the committee recommended the development of success criteria for the EBR-II spent fuel demonstration project: “A well-defined set of performance criteria needs to be developed. The criteria would provide ANL with a clear set of objectives. The achievement of those objectives would better position ANL to request approval to proceed to additional applications of its electrometallurgical technology program.”3 This 1 See Appendix D, in which are reprinted the recommendations made in the committee’s nine reports. 2 National Research Council, An Assessment of Continued R&D into an Electrometallurgical Approach for Treating DOE Spent Nuclear Fuel, National Academy Press, Washington, D.C., 1995, pp. 5-7 and 5-8. 3 National Research Council, Electrometallurgical Techniques for DOE Spent Fuel Treatment: Fall 1996 Status Report on Argonne National Laboratory’s R&D Activity, National Academy Press, Washington, D.C., 1996, p. 7.
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report point was reiterated in the committee’s sixth report: “Before the demonstration is completed, DOE should establish criteria for success in the demonstration phase to allow evaluation of the electrometallurgical technology for further use.”4 The criteria proposed by the committee were based on what the committee believed were reasonable estimates of a pilot-plant-scale production. In preparation for operations related to the spent fuel demonstration project, ANL prepared an Operation Readiness Review for the fuel conditioning facility (FCF) where radioactive operations were to take place.5 In August 1995, the DOE Material Control and Accountability Audit was completed.6 During the summer of 1995, several nongovernmental organizations had questioned the adequacy of the environmental assessment (EA) prepared under the IFR program. The resolution of environmental issues was all that was needed before operations with irradiated fuel could begin. During the fall of 1995, ANL decided to prepare a new environmental impact assessment to specifically address the spent fuel treatment operations in the FCF. This document was issued by DOE during late January 1996,7 and the environmental evaluation was completed in the spring of 1996. As a result of the new EA, the demonstration project was scaled back from initial estimates. The goal was to process 100 driver and 25 blanket fuel assemblies from EBR-II to demonstrate the electrometallurgical technique.8 In 1998, ANL proposed a set of performance criteria for the demonstration project, with goals to meet each criterion. The committee in its seventh report evaluated these criteria and goals and found them to be adequate for assessing the success of the demonstration project.9 DEMONSTRATION PROJECT SUCCESS CRITERIA The criteria proposed by ANL in 1998 for the demonstration project were similar in scope to those recommended by the committee in 1995, but smaller in scale in order to conform to the EA. The four criteria address the process, the waste streams, and the safety of the electrometallurgical demonstration project. The four criteria and lists of goals are reprinted, with the exception noted, from pages 24 and 25 of the committee’s seventh report. Criterion 1: Demonstration that 100 driver and up to 25 blanket experimental breeder reactor assemblies can be treated in a fuel-conditioning facility (FCF) within 3 years, with a throughput rate of 16 kg per month for driver assemblies sustained for a minimum of 3 months and a blanket throughput rate of 150 kg per month sustained for 1 month.10 4 National Research Council, Electrometallurgical Techniques for DOE Spent Fuel Treatment: Status Report on Argonne National Laboratory’s R&D Activity Through Spring 1997, National Academy Press, Washington, D.C., 1997, p. 11. 5 K.M. Goff, R.D. Mariani, D. Vaden, N.L. Bonomo, and S.S. Cunningham, “Fuel Conditioning Facility Electrorefiner Start-up Results,” in Proceeding of the Embedded Topical Meeting on DOE Spent Nuclear Fuel & Fissile Material Management, Reno, NV, June 16-20, 1996, American Nuclear Society, Inc., La Grange Park, IL, pp. 137-143. 6 Environment, Safety, and Health, Material Control and Accountability Manual, Lawrence Livermore National Laboratory, Livermore, CA, 1995. 7 U. S. Department of Energy, Draft Environmental Assessment – Electrometallurgical Treatment Research Demonstration Project in the Fuel Conditioning Facility at Argonne National Laboratory-West, DOE/EA-1148, Washington, D.C., 1996. 8 In June 1999, Robert G. Lange, associate director for Nuclear Facilities Management, Office of Nuclear Energy, Science and Technology, sent a letter to the National Research Council, clarifying the amount of EBR-II spent fuel that was treated in the demonstration project. In this letter Lange states that “The Finding of No Significant Impact issued in May 1996 for the environmental assessment of the demonstration project was based on the treatment of no more than 125 assemblies of EBR-II spent fuel (100 driver assemblies and 25 blanket assemblies).” 9 R.W. Benedict, H.F. McFarlane, J.P. Ackerman, R.K. Ahluwalia, L.L. Briggs, H. Garcia, E.C. Gay, K.M. Goff, S.G. Johnson, R.D. Mariani, S. McDeavitt, G.A. McLennan, C. Pereira, P.D. Roach, and B.R. Westphal, Spent Fuel Treatment Demonstration Interim Status Report, NT Technical Memorandum No. 74, Argonne National Laboratory, Argonne, IL, 1998, Appendix A. 10 The original statement of this criterion was as follows: “Demonstration that 125 EBR-II assemblies can be treated in a fuel-conditioning facility (FCF) within 3 years with a throughput rate of 16 kg/month for driver assemblies sustained for a minimum of 3 months and a blanket throughput rate of 150 kg per month sustained for 1 month.” The intent of this success criterion was to define minimum required throughput rates for the treatment process to be met within 3 years using no more than the amount of EBR-II fuel that had been set aside. All 100 drivers
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report Specific goals to meet criterion 1: Freeze process modifications and operating parameters while demonstrating a continuous throughput of 16 kg of driver uranium for 3 consecutive months. Demonstrate the capability to electrorefine approximately 150 kg of blanket spent fuel in 1 month. Distill the electrolyte from ER cathode products through the cathode processor in an FCF and blend the resulting ingot with depleted uranium in the casting furnace to produce a low-enriched uranium storage ingot. Specify acceptable operating parameters and throughput for the cathode processor to meet uranium product specifications and ER production rates of 16 kg of driver uranium for 3 consecutive months. Specify acceptable casting-furnace operating parameters for producing low-enriched uranium from 16-kg driver uranium per month for 3 consecutive months. Cast three batches of irradiated cladding hulls (two driver assemblies per batch) into a typical metal waste form (stainless steel with 15 percent zirconium). Process 3 kilograms of salt containing approximately 6 wt % fission products into 10 ceramic waste samples. Criterion 2: Quantification (for both composition and mass) of recycle, waste, and product streams that demonstrate projected material balance with no significant deviations. Specific goals to meet criterion 2: Develop uranium product specifications with range of acceptable impurities: plutonium, neptunium, technetium-99 and ruthenium-106. Specify process-operating parameters for uranium ingots that meet uranium specifications. Develop metal waste specifications that are based on performance characterization results of small samples with variations in the principal constituents: zirconium, uranium, technetium, plutonium, neptunium, and noble metals. Determine performance characterization with electrochemical technique, corrosion tests, vapor hydration tests, and attribute tests. Develop metal waste process specifications for major process variables: operating temperatures, hold time, and cooling rate. Develop ceramic waste specifications that are based on performance characterization results of samples with principal constituent variations: glass, fission products, uranium, and plutonium. Determine performance characteristics with attribute, characterization, accelerated, and service condition tests. Develop ceramic waste process specifications for major process variables: free chloride, zeolite moisture content, and chloride per unit cell. Quantify volume of low-level and transuranic waste generation under standard operating conditions. Return the cathode processor condensate to the individual ERs during the 16-kg driver per month for 3 months and 150 kg blanket per month operations. Specify unit process operations for metal spent fuel treatment, uranium ingot production, and waste form production. Estimate mass balances for uranium, transuranics, sodium, and key fission products for overall process. Prepare the flowsheet and develop process specifications for the subsequent inventory operation. were treated to produce the needed throughput data and to obtain the fission product buildup required to test ceramic waste form production. However, it was projected that throughput and performance goals under this criterion for the blanket fuel would be met before 25 blanket assemblies would have been treated. Therefore, to ensure that this intent was properly understood, DOE recommended the change in wording for success criterion 1. The committee agreed with this change in wording.
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report Criterion 3: Demonstration of an overall dependable and predictable process, considering uptime, repair and maintenance, and operability of linked process steps. Specific goals to meet criterion 3: Record facility and equipment availability for process operations during the 3-month 16 kg per month driver demonstration. Record process interruption for chemistry results during the 3-month operation at 16 kg per month. Develop quantitative process models for each key step in the treatment process. Develop a process model that estimates throughputs as a function of equipment availability, maintenance requirements, and individual process times. Criterion 4: Demonstration that safety risks, environmental impacts, and nuclear materials accountancy are quantified and acceptable within regulatory limits. Specific goals to meet criterion 4: Demonstrate that the FCF air emissions result in an effective dose equivalent to the public less than 10 mrem per year, which is the limit in DOE 5400.5 and is less than the 25 mrem per year limit in the State of Idaho Permit to Construct Air Pollution Emitting Source. Show that FCF personnel exposure is less than 0.5 rem per year average and 1.5 rem per year for the maximum individual exposure, which is a factor of 3 less than the DOE Occupational Radiation Protection Final Rule 10CFR835 limit that is 5 rem per year. Demonstrate a material control and accountability system that shows the historical inventory difference for uranium and plutonium is within control limits based on variance propagation of measurement and sampling errors, as specified in DOE Order 5633.3B. Record any unlikely and extremely unlikely accident (as defined in the Final Safety Analysis Report) during the demonstration. Estimate the safety risks, environmental impacts, and material accountancy for the inventory operations. COMMITTEE EVALUATION OF ANL’S DEMONSTRATION PROJECT BASED ON THE DEMONSTRATION PROJECT SUCCESS CRITERIA The committee’s evaluation of ANL’s ability to meet the demonstration project success criteria derived from a number of factors. The committee received technical memoranda from ANL covering all aspects of its demonstration project. The committee also made yearly visits to both ANL-W, where the demonstration project took place, and ANL-E, where R&D was performed in support of the demonstration project. The committee also met with ANL personnel involved in the demonstration project in formal briefings at least three times each year. All of these sources of information were utilized in the committee’s evaluation. After the demonstration project was completed, the committee received a final overview of the technical accomplishments of the electrometallurgical demonstration project from Robert Benedict (ANL) in September 1999.11 This briefing included the release to the committee of ANL final reports on the demonstration project. Following the September 1999 briefing, the committee reviewed each of the success criteria, together with each related goal to meet the success criteria, in order to come to an overall evaluation of the electrometallurgical demonstration project. The committee came to the following conclusions: 11 See summary in Appendix C.
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report Criterion 1 Goal 1: The committee believes that this goal has not only been met, but the rate of processing has been exceeded. Goal 2: The committee believes that this goal has been met. Goal 3: The committee believes that this goal has been met. Goal 4: The committee believes that this goal has been met.12 Goal 5: The committee believes that this goal has been met. Goal 6: The committee believes that this goal has been met noting that the actual content of the as-produced ingots fits the target range of 5 to 20 percent Zr. Goal 7: The committee believes that this goal has been met. Criterion 2 Goal 1: The committee believes that this goal has been met. Goal 2: The committee believes that this goal has been met. The committee notes that these are not results, they are methods. Goal 3: The committee believes that this goal has been met. Goal 4: The committee believes that this goal has been met. The committee notes that testing time has been limited. This statement is made not as a criticism, but as an observation. Although the committee believes that this goal has been met, this conclusion does not imply that either the metal waste form or the ceramic waste form are qualified waste forms. In addition, the committee recognizes that further data collection and analysis must be carried out in the post-demonstration period to support a final decision on MWF and CWF acceptability for repository disposal. Goal 5: The committee believes that this goal has been met. For movement to larger HIP cans, further R&D is needed in the post-demonstration period. The process referred to in the goal is for small HIP cans. Goal 6: The committee believes that this goal has been met. Goal 7: The committee believes that this goal has been met. Goal 8: The committee believes that this goal has been met. Goal 9: The committee believes that this goal has been met. The committee notes that the data for the driver fuel is more important than the data for the blanket fuel. Goal 10: The committee believes that this goal has been met. Criterion 3 The committee notes that the demonstration was limited to a relatively short period at the end of the demonstration project period, as much of the early period of the overall demonstration project was spent on R&D. Goal 1: The committee believes that this goal has been met. Goal 2: The committee believes that this goal has been met. Goal 3: The committee believes that this goal has been met. Goal 4: The committee believes that this goal has been met. Criterion 4 Goal 1: The committee believes that this goal has been met. Goal 2: The committee believes that this goal has been met. 12 A full description of the results obtained to meet this goal may be found in H.F. McFarlane, K.M. Goff, T.J. Battisti, B.R. Westphal, and R.D. Mariani, Options for Disposition of Uranium Recovered from Electrometallurgical Treatment of Sodium-Bonded Spent Nuclear Fuel, NT Technical Memorandum No. 109, Argonne National Laboratory, Argonne, IL, 1999.
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report Goal 3: The committee believes that this goal has been met. Goal 4: The committee believes that this goal has been met. Goal 5: The committee believes that this goal has been met, based on ANL’s safety analysis.13 Concerns with scale-up of the HIP process have been noted by the committee in previous reports.14 Findings and Summary Finding: The committee finds that ANL has met all of the criteria developed for judging the success of its electrometallurgical demonstration project. Finding: The committee finds no technical barriers to the use of electrometallurgical technology to process the remainder of the EBR-II fuel. The EBR-II demonstration project has shown that the electrometallurgical technique can be used to treat sodium-bonded spent fuel. If the DOE decides to complete the treatment of EBR-II spent fuel and blanket material, the committee has found that there are no technical barriers to the use of EMT to achieve this objective. The major hurdle that remains is qualification of the waste forms from this processing. The total quantity is relatively small, particularly in comparison to the total DOE spent fuel inventory, so even if qualification of the waste form were to prove impossible, the quantity of these materials that had been produced would be modest. The committee has found no significant technical barriers in the use of electrometallurgical technology to treat EBR-II spent fuel, and EMT therefore represents a potentially viable technology for DOE spent nuclear fuel treatment. However, before using EMT for processing other spent fuels in the DOE inventory that would generate much larger amounts of these wastes than were produced in ANL’s demonstration project, it would be necessary for these waste forms to receive the acceptance qualification. 13 H.E. Garcia, C.H. Adams, D.B. Barber, R.G. Bucher, I. Charak, R.J. Forrester, S.J. Grammel, R.P. Grant, R.J. Page, D.Y. Pan, A.M. Yacout, L.L. Burke, and K.M. Goff, Analysis of Spent Fuel Treatment Demonstration Operations, NT Technical Memorandum No. 108, Argonne National Laboratory, Argonne, IL, 1999. 14 National Research Council, Electrometallurgical Techniques for DOE Spent Fuel Treatment: Status Report on Argonne National Laboratory’s R&D Activity as of Fall 1998, National Academy Press, Washington, D.C., 1999, p. 19.
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