Nuclear Applications of Accelerators; Experience in the 'A' Programs (APT, ATW, AAA, AFCI)

1. LA-UR 09-00879 Nuclear Applications of Accelerators; Experience in the 'A' Programs (APT, ATW, AAA, AFCI) Dr. Laurie Waters Group D-5, International Nuclear & Systems AnalysisLos Alamos National Lab February 12, 2009 Fermi National Laboratory

2. High Power, High Energy, Industrial Accelerators • Accelerator Production of Tritium • Accelerator Transmutation of Waste • Advanced Accelerator Applications (ADTF) • Accelerator Driven Systems • Advanced Fuel Cycle Initative • Power production • Radioisotope Production

3. High Power Accelerators * * Beam Power (MW) = Energy (MeV) x Current (Amps)

4. Planned Facilities • LEDA

5. Tritium Production in the US (Tritium halflife is 12.3 years) • 1953-1955 Tritium producing reactors online • 1976-1988 Need for new tritium production method recognized, many false starts, controversy, no real progress • 1979 Three Mile Island • 1986 Chernobyl • 1987 N and C reactors shutdown • 1988 K, L and P shutdown • 1989 Plan to refurbish/restart K New Production Reactor (NPR) project start - MHTGR (modular hi-temp gas- • cooled reactor), HWR, LWR • 1990 Ebasco HWR and MHTGR selected • 1991 Arms reduction progress, only one option needed. K reactor leaks. • 1992 $1.5B spent on K reactor $1.5B spent on NPR, program cancelled • 1993 K reactor restart cancelled • 1995 APT primary option, and CLWR is the backup • 1997 TVA proposed sale of of Bellefonte to DOE with Watts Bar/Sequoya service as backup • 1998 “Interagency review” issued Watts Bar service chosen

6. DOE Dual Track Tritium Strategy DOE Tritium Production Options in December 1995 Purchase Irradiation Services or Commercial Reactor Build Advanced Light WaterReactor (Small or Large) Build Modular High TemperatureGas-Cooled Reactor (MHTGR) Build Heavy Water Reactor (HWR) Build Proton Accelerator (APT) system Accelerator APT Backup CLWRPrimary DOE Decision 12/1998 CommercialReactor Option(s) TVA Watts Bar and Sequoyah Power Reactors • 10a

7. Extensive Testing of the Prototype Proton Injector Shows its Suitability for APT Operations Beam transport 350 MHz 700 MHz RF Systems RFQ CCDTL CCL SCL (ß = 0.64) SCL (ß = 0.82) Injector • The injector produces the proton beam and gives it an initial energy of 75 keV. • The APT injector prototype has demonstrated >110 mA of proton current at 75 keV, with exceptionally good properties and 96% - 98% availability. 97 MeV 211 MeV 471 MeV 1030 MeV 1700 MeV 100 mA TSF Beamstop T/B

8. The APT Radio Frequency Quadrupole is Similar to Others Used in Accelerators Worldwide Beam transport 350 MHz 700 MHz RF Systems RFQ CCDTL CCL SCL (ß = 0.64) SCL (ß = 0.82) Injector • The 8-m long RFQ bunches the beam and gently accelerates to 6.7 MeV • It has 4 tuned segments, is an all-brazed structure, of copper, resonance control by water temperature. • The RFQ has met the project milestone of extended cw operation at 100 mA. 97 MeV 211 MeV 471 MeV 1030 MeV 1700 MeV 100 mA TSF Beamstop T/B Waveguide Support Structure RFQ

9. Normal-Conducting Copper Accelerating Structures Will Take the Beam from 6.7 to 211 MeV Beam transport 350 MHz 700 MHz RF Systems RFQ CCDTL CCL SCL (ß = 0.64) SCL (ß = 0.82) Injector • Normal-conducting copper structures are used to accelerate the beam to 211 MeV • A coupled cavity drift tube linac (CCDTL) will be used to 100 MeV. • The section from 100 MeV to 211 MeV will be a coupled-cavity linac similar to the installation at Fermilab shown on the right • Prototype cavities are under fabrication 97 MeV 211 MeV 471 MeV 1030 MeV 1700 MeV 100 mA TSF Beamstop T/B Fermilab

10. Superconducting Niobium Cavities Take the Beam from 211 MeV to 1030 MeV Beam transport 350 MHz 700 MHz RF Systems RFQ CCDTL CCL SCL (ß = 0.64) SCL (ß = 0.82) Injector • Repetitive sets of niobium cavities are used to accelerate the beam to the full energy. • The use of superconducting niobium saves 20% of the capital and electric power cost. • The APT design allows the use of only two cavity shapes, simplifying manufacturability and lowering cost. 97 MeV 211 MeV 471 MeV 1030 MeV 1700 MeV 100 mA TSF Beamstop T/B  = 0.64 Cryomodule Vacuum Jacket Waveguide 5 -cell Nb Cavity Power Coupler

11. Highly Efficient RF Generators Will Power the Plant Beam transport 350 MHz 700 MHz RF Systems RFQ CCDTL CCL SCL (ß = 0.64) SCL (ß = 0.82) Injector • Radio Frequency power to accelerate the beam is supplied by klystrons • Three 1.2-MW, 350 MHz supplies have been installed to run the RFQ at LEDA • Two 1-MW, 700 MHz tubes for the rest of the accelerator are in operation 97 MeV 211 MeV 471 MeV 1030 MeV 1700 MeV 100 mA • TSF Beamstop T/B 350 MHZ, 1.2 MW Klystron

12. The Target/Blanket Produces Tritium Efficiently Using a Tungsten and Lead Neutron Source Beam transport 350 MHz 700 MHz RF Systems RFQ CCDTL CCL SCL (ß = 0.64) SCL (ß = 0.82) Injector • The Target/Blanket efficiently produces and converts 3He into tritium • The system operates at low temperature and pressure • The modular design allows periodic replacement of components • Tritium inventory is minimized by semi-continuous removal 97 MeV 211 MeV 471 MeV 1030 MeV 1700 MeV 100 mA TSF Beamstop T/B Lead Blanket Modules Cavity Vessel Iron Shield Window Tungsten Neutron Source Proton Beam

13. Tritium Separation Facility Recovers Tritium from Helium, Separates Tritium from Protium, and Ships Product Beam transport 350 MHz 700 MHz RF Systems RFQ CCDTL CCL SCL (ß = 0.64) SCL (ß = 0.82) Injector 97 MeV 211 MeV 471 MeV 1030 MeV 1700 MeV 100 mA TSF Beamstop T/B Remove spallation and activation products from gas Recover hydrogen isotopes using palladium-silver permeators Separate tritium from protium using cryogenic distillation Package/ship tritium to SRS Tritium Facilities in DOT package Supply purified 3He to Target/Blanket Confine systems in gloveboxes to minimize environmental releases Tritium Processing Glovebox

14. DOE Dual Track Tritium Strategy DOE Tritium Production Options in December 1995 • Accelerator • Purchase Irradiation Services or Commercial Reactor • Build Advanced Light WaterReactor (Small or Large) • Build Modular High TemperatureGas-Cooled Reactor (MHTGR) • Build Heavy Water Reactor (HWR) • Build Proton Accelerator (APT) system • APT Backup • CLWRPrimary • DOE • Decision • 12/1998 • CommercialReactor Option(s) • TVA Watts Bar and Sequoyah Power Reactors • 10a

15. The APT Mission as Backup is to Complete ED&D and Preliminary Design of a Modular Plant • Heat Exchanger • Maintenance Building • Klystron Gallery • Injector • Cryogenics Plant • Tritium Separation Building • 1030 MeV Transport Line • 1700 MeV Transport Line • The Modular Design APT Plant features: 1.5 kg/year plant capacity with an option (shown) for an upgrade to a plant capacity of 3 kg/year or downgrade to 1 kg/year. Design Target/Blanket and Tritium Processing for a maximum capacity of 3 kg/year • Target/Blanket Building

16. Materials HandbookRevision 5, June 2006 • Alloy 718 • 316L Stainless Steel • 6061 Aluminum • 316L to 6061-T6 Aluminum welds • Lead • Niobium • Graphite • RF Window Alumina • Tritium systems materials, coolants, fluids • 304L Stainless Steel • 9Cr-1Mo Ferritic/Martensitic Steel (T91) • Tantalum • Lead-Bismuth Eutectic

17. Mechanical Property Data Needed • Al6061-T6 In Beam Mechanical Property data needed Rung materials Alloy 718 Superplastic form Alloy 718 Annealed Clad materials Alloy 600 Annealed 316L annealed Tungsten Alloys (comp/bend) CVD W-PS & forged W with La2O3 W-wrought HIPPED Bonds Thermal Conductivity Test-pure materials Bond measurements ultrasonic measurements before/after measure using thermogravimetric camera Weld Materials SS-3 tensile, cut directly out of weld Compact Tension ? 316/316, 718/718, Fatigue Crack Growth (FCG) specimens 316L, Alloy 718 CT type specimens Prestrained (PS) materials Alloy 718-SP Tensile • Corr • WComp • WBend • 718SP • Corr Out of Beam Mechanical Property data needed Al6061 (T6, T4?) fracture toughness tensile (high dose) Al/SS Inertial welds, Al/Al welds fracture toughness tensile Fatigue Crack Growth specimens Al6061-T6 • Alloy 600 • WComp • WBend • 718Ann • FCG 718 Ann • Weld SS-3 • Corr • Corr • Corr • Corr • Weld SS-3 • Weld SS-3 • 718SP-PS • Al 6061-T6 • FCG 316L • TC pure mat or Al6061-T6 FCG • Corr • Weld SS-3 • Smart/Opt mat. • Weld SS-3 • Al6061-T6 • Al6061-T6 FCG

18. Tungsten Example results

20. Corrosion rates (SS316L)Electrical Impedance Spectroscopy with corrosion probes

21. Effect of beam structure

22. Materials Test Station Baseline Design • Monolithic design using HT-9 is main structural material and is Pb-Bi and D2O cooled. • A split proton beam impinges on two targets, providing a center flux trap for fuel irradiations. • Materials samples will be placed on the outsides of the targets. • Target will be driven by 800-MeV, 1.35-mA proton beam. • Operation at 75% capacity factor for 8 months of the year (4400 h/yr)

23. The MTS target design will serve as a fast-flux irradiation facility for nuclear fuel and materials. • The center flux trap will see a peak of 1.5x1015 n/cm2/s total flux (and 1.3x1015 n/cm2/s fast flux). • Fuel clad temperatures will be near-prototypic (400-500C) • Materials samples can be placed in the side modules which see less flux intensity but will have limited active temperature control. • The high-energy tail from the spallation interactions will increase the He/dpa ratio depending on location in the target.

24. Facility Layout Protonbeam

25. Proton Flux

26. Neutron Flux • Neutron flux at the midplane varies from ~5 x 1014 to almost 1.3e15 n/cm2/s.

27. Point Defect Measurement

28. Comparisons with NRT and Molecular Dynamics (MDCASK)

29. Decay Heat Measurement

30. Comparison of measured and calculated decay heat

31. The PMMA/Goodman Liquid Water PhantomTissue-Equivalent Ion Chambers

32. Measured Neutron Spectra at the Phantom

33. Nuclear Fuel Cycle

34. Two Criteria support Enhance Long-Term Public Safety Reduction in Predicted Dose by 99% requires: Neptunium chain (245Cm, 241Pu, 241Am, 237N) reduction by 99.5 - 99.8% Actinium chain (243Cm, 243Am, 239Pu ) reduction by 99.6 -99.9% Radium Chain (242Pu, 238Pu, 234U) reduction by 98.9 - 99.6% Thorium Chain (244Cm, 240Pu) reduction by 99.3 - 99.7%

36. US DOE AAA Program Developing Lead-Bismuth Eutectic Technology for High-PowerSpallation Neutron Targets N. Li, K. Woloshun, V. Tcharnotskaia, C. Ammerman, T. Darling, J. King, X. He, D. Harkleroad The U.S. DOE Advanced Accelerator Applications (AAA) Program aims to develop an Accelerator-Driven Test Facility (ADTF) that provides a world-class test facility to assess technology options for the transmutation of spent nuclear fuel and waste, and provide a test bed for advanced nuclear technologies and applications. The development and testing of a high power high flux spallation target as the external neutron source for the subcritical blanket is critical for ADTF and future Accelerator-driven Transmutation of Waste (ATW) applications. Lead-bismuth eutectic (LBE) emerged as a leading candidate for high-power spallation targets. LBE has exceptional chemical, thermal physical, nuclear and neutronic properties well suited for nuclear coolant and spallation target application. The Materials Test Loop (MTL) is an essential part of the out-of-beam testing program in the U.S. MTL is a major step toward demonstrating the use of LBE on a scale representative of MW level spallation targets.

37. Active control of oxygen in LBE can prevent steel corrosion and coolant contamination N. Li, “Active Control of Oxygen in Molten Lead-Bismuth Eutectic Systems to Prevent Steel Corrosion and Coolant Contamination”, LA-UR-99-4696, to appear in Journal of Nuclear Materials

38. Achievable Reduction of Corrosion and Precipitation through Active Oxygen Control X.Y.He, N. Li and M. Mineev, “A Kinetic Model for Corrosion and Precipitation in Non-isothermal LBE Flow Loop”, Journal of Nuclear Materials 297 (2001) 214-219 Corrosion/precipitation rate in the MTL with oxygen control and without oxygen. Rates for oxygen controlled LBE are multiplied with 100 and 1000 respectively for two oxygen levels.

39. MTL DAC Front Panel MTL Upper Loop Section MTL Heater Section MTL Front View

40. Isotope Production Facility at LANSCE • Fall 2003, new facility • 100 MeV H+ beam, up to 200 microamps • Aluminum 26 (aluminum tracer), Silicon 32 are unique to LANL • Strontium-82 is supplied to GE Healthcare for use in the CardioGen(r) rubidium-82 generator. The generators in turn are supplied to hospitals and medical laboratories to support cardiac imaging through Positron Emission Tomography (PET). The generator technology was developed by the DOE Medical Radioisotope Program during the 1970s and 1980s, and the technology was transferred to private industry in the late 1980s. The DOE continues to be one of the principle suppliers of the strontium-82 for the generators. Strontium-82 is produced by bombarding rubidium chloride or rubidium metal with protons with energies between 40 and 70 MeV. • Germanium-68 is used for calibration sources for medical imaging equipment. Hospitals and research institutions across the nation use such sources every day to calibrate PET scanners. Without such calibrations the usefulness of equipment for medical imaging and research would be severely limited. Germanium-68 is produced by bombarding gallium metal with protons with energies between 20 and 70 MeV. • Silicon-32 is used in oceanographic research to study the silicon cycle in marine organisms, principally diatoms. Its use in this application has dramatically improved the timeliness and quality of data available in this area of environmental research. Silicon-32 is produced by high-energy (> 90 MeV) proton bombardment of sodium chloride.

41. Regulatory considerations • Accelerator-driven attractive because of ‘inherent safety’ • Subcritical systems • Turn off the beam, problem goes away • Don’t get out of extensive safety analysis. • 10CFR831

42. Funding • GNEP (Global Nuclear Energy Partnership) • Int’l partnership to promote the use of nuclear power and close the nuclear fuel cycle to reduce waste and proliferation risk. ‘Bypass’ Yucca Mountain. • Promoted fast reactor technology, but didn’t go over well with the utilities (who want to concentrate on GEN3 reactors). • No demonstration projects • Basically dead • Advanced Fuel Cycle Initiative (AFCI) • Focused R&D effort • Develop fuel systems for GEN IV reactors • Reduce high level waste volume • Greatly reduce long-lived and highly radiotoxic elements • Relcaim energy content of spent nuclear fuel