HFIR and Isotope Production

Transcription

1 HFIR and Isotope Production Presented to the National challenges to elimination of HEU in civilian research reactors David J. Dean Director, Physics Division Isotope Program Director Washington, DC April 3, 2017 ORNL is managed by UT-Battelle for the US Department of Energy

2 Outline ORNL s role in the DOE Isotope Program HFIR and isotope applications HEU to LEU and HFIR (redux) Questions APS/POPA

3 ORNL s role in the DOE Isotope Program

4 DOE Isotope Program Managed by the Office of Nuclear Physics in the Office of Science Mission: Produce and/or distribute radioactive and stable isotopes that are in short supply, associated byproducts, surplus materials and related isotope services Maintain the infrastructure required to produce and supply isotope products and related services Conduct R&D on new and improved isotope production and processing techniques which can make available new isotopes for research and applications. Recommendations of the 2015 Isotope Long Range Plan Significant increase in R&D funding Alpha emitters Reactor and accelerator target development HSA theragnostics Full intensity operations of the stable isotope separation capability Increase in annual appropriations Radioactive isotope separations FRIB separations BNL (BLIP) and LANL (IPF) upgrades Other recommendations included continued workforce development APS/POPA

5 Facilities supporting DOE Isotope Program APS/POPA

6 DOE Isotope Program funding and engagement Statutory Authority: Public Laws (1990) and (1995) The annual appropriation in NP funds a payment into the revolving fund to Collections from isotope sales Annual Appropriations Community Engagement Maintain mission-readiness by supporting the core scientists and engineers needed to carry out the IP Maintain isotope facilities to assure reliable production Provide support for R&D activities associated with development of new production and processing techniques for isotopes, production of research isotopes, and training of new personnel in isotope production In FY 2015, a total of $53M was deposited in the revolving fund Appropriation of $20M paid into the revolving fund from the Nuclear Physics program ($4.9M in research) Collections of $33M to recover costs related to isotope production and isotope services DOE IP community engagement: Isotope Program Operations DOE/SC/NP Annual strategy meetings Stakeholder meetings Federal Workshop DOE/NIH meetings National Isotope Development Center APS/POPA NSAC

7 The ORNL Isotope Program Strategy Vision The ORNL Isotope Program will be sustainable and always improving provide a high ratio of societal benefit to taxpayer investment deliver high-quality, relevant applied research be recognized as a desirable partner to the applications and research and development community. ORNL assets People with significant experience in each area we are pursuing Nuclear Infrastructure: HFIR, radiochemistry expertise, hot cells, transportation expertise Certifications for stable isotope distribution (e.g., ISO-9001) Extremely supportive senior management Outcome: Full utilization of the unique resources at ORNL to meet DOE needs for isotope products and services which are beyond the means of commercial enterprises Strategy Maintain and enhance our infrastructure to ensure that commitments for the production of stable and radioactive isotopes are met safely and reliably Develop a vibrant isotope research effort that disseminates results through publications and enables future production Coordinate and integrate NP isotope effort with Pu-238 and other key isotope work at ORNL Provide a meaningful path toward succession and workforce development within the isotope effort APS/POPA

8 HFIR and isotope applications

9 How to make isotopes Blow things up (not a good idea) Irradiate existing isotopes Neutron capture in a reactor (ORNL, INL, MURR) Proton or light-ion reactions in an accelerator (LANL, BNL) Chemical separations (nuclear chemistry) Almost every production method relies on chemical separations Harvest isotopes from Cold War surplus material Mechanical separations Stable isotope production with electromagnetic or centrifuge technology (or diffusion) Import (Russian) But APS/POPA

10 High Flux Isotope Reactor Is a Unique Facility with Multiple Missions Versatile 85 MW Reactor Highest thermal flux in Western world 2.5E15 n/cm 2 -s thermal 1.2E15 n/cm 2 -s fast Neutron Scattering Research Brightest cold neutron source in world Isotope Production Material Irradiation Neutron Activation Analyses Neutrino R&D APS/POPA Operations: SC/BES

11 ORNL Radioisotopes APS/POPA

12 HFIR produces diverse isotopes for a variety of applications Energy Industrial Security Medical Mineral analyzers Cancer Treatments Nuclear fuel quality control Reactor start-up sources Coal analyzers Oil exploration Cement analyzers FHA measurements for corrosion (bridges, highway infrastructure) Handheld contraband detectors (CINDI) Standard for all neutron fission measurements Monitoring downblending of HEU Identifying unexploded chemical ordnance and detecting land mines APS/POPA Mars Rover Curiosity uses an RTG containing 3.6kg 238 Pu to produce electricity. -NASA image

13 Radioisotope production at ORNL 252 Cf 63 Ni 75 Se 225 Ac 212 Pb 188 W 227 Ac 89 Sr 109 Cd 133 Ba 14 C ORNL also dispenses high purity 242 Pu, 234 U, 239 Pu, and 243 Am from inventory APS/POPA

14 Example: Cf-252, many industrial and research apps 100 Fm Fm 254 Fm 255 Fm 256 SF Fm Es Es 253 Es 254 Es 255, -, EC - 98 Cf Cf 249, (n,f) Cf 250 Cf 251 Cf 252 Cf 253 Cf 254, (n,f), SF -, (n,f) SF Feedstock (heavy curium) in place for 15+ years DOE produces at ORNL for a consortium Variety of uses Z Pu Np 96 Cm 95 Am 97 Bk Cm 242 Cm 243 Cm 244 Cm 245 Cm 246 Cm 247, (n,f), (n,f), (n,f) Am 241 Am 242 Am 243 Am 244 Am 245 Am 246 -, EC Pu 238 Pu 239 Pu 240 Pu 241 Pu 242 Pu 243 Pu 244 Pu 245 Bk Cm 248, SF Pu 246, (n,f) -, (n,f) Np 237 Np 238 Bk 250 Bk Cm 249 Cm SF APS/POPA N

15 Contribution to nuclear physics R&D CARIBU Sources 3 mci (2008); 100 mci (2009) 500 mci (2012) 1.7 Ci Cf-252 (Nov, 2013) Neutron rich physics reach Nuclear astrophysics Superheavy Elements Bk and Cm sources for Ca-48 beams at Dubna Discovery of A= APS/POPA

16 Naming of element 117 Tennessine (Ts) (and we are not done with new element discoveries) 28 th November 2016 Gov. Bill Haslam (left) speaks with Wigner Lecturer Yuri Oganessian at Jan. 27's lecture and reception. In the background are (from left) DOE's Timothy Hallman, Sergey Dmitriev of the Russian Joint Institute for Nuclear Research, JINR Director Victor Matveev and ORNL Director Thom Mason. (ORNL Today) APS/POPA Bk-249 targets produced at HFIR

17 It takes time to develop isotopes: The story of 82 Sr/ 82 Rb Chatal J-F, Rouzet F, Haddad F, Bourdeau C, Mathieu C and Le Guludec D (2015) Story of rubidium-82 and advantages for myocardial perfusion PET imaging. Front. Med. 2:65. doi: /fmed : studies in dogs (Love et al., Cir. Res. 2, 112 (1954)) Myocardial uptake directly proportional to myocardial blood flow (MBF) Clinical studies in the 1980s Approval for use in the US in Rb PET has better diagnostic accuracy than 99mTc-SPECT especially in obese patients To be economically viable, an accelerator with proton beam of energy higher than 70 MeV and intensity >100 µa must be used. There are only few places in the world where such accelerators are available: Brookhaven National Laboratory (BNL-USA), Los Alamos National Laboratory (LANL-USA), ithemba labs (South Africa), INR (Russia), Triumf (Canada), and Arronax (France) APS/POPA Accelerator example. Applies to reactor production as well

18 Targeted alpha therapy in theory High-linear-energy α-particle emissions create dense ionization paths in tissue that render high target-to-nontarget dose ratios that are highly effective at cell killing George Sgouros, SNNMI-MIRD, 2015 The therapeutic outcome of TAT is influenced by a number of crucial issues that all need to be handled, e.g., the specificity of the antibody/targeting construct; the level of antigenic expression on the tumor cells; the potential loss of immunoreactivity of the antibody/targeting construct; the amount of unlabeled antibody/targeting construct after injection; the existence of diffusion barriers that hinder the penetration of the antibody/ targeting construct into the tumors; the choice of radionuclide (half-life and path length); too low specific radioactivity; and for the i.p. situation, any extra peritoneal location of tumor cells. (Elgqvist) Elgqvist et al., Front. Oncol. 3, 324 (2013) µm APS/POPA

19 Alpha therapy in practice: 223 Ra Xofigo (radium-223 dichloride, Bayer)- First FDA Approved Alpha Therapy Agent in 2013 Ra-223 (t 1/2 = d; multiple α particles between 5-6 MeV) Used to treat bone metastases in end-stage prostate cancer Radium is preferentially absorbed by bone by virtue of its chemical similarity to calcium Naturally targets new bone growth in and around bone metastases Therapeutic effect is largely palliative, it is not targeted Paves the way for other alpha therapy agents Before treatment (left) and after 6 cycles of Ra-223 (right) APS/POPA

20 Alpha emitters APS/POPA Issues Short half lives (production) Associated chemistry (how to get into the body) Toxicity (bi products)

21 PROSPECT Motivations and Goals PROSPECT is a DOE (HEP)-funded multi-phase shortbaseline reactor experiment that will be installed at the High Flux Isotope Reactor (HFIR). Antineutrino flux observed vs model. (PRL116, ) The Flux Deficit Previous reactor experiments observed a 6% flux deficit when compared to reactor models. Physics Goal 1: Search for short-baseline oscillations and conclusively address the sterile neutrino hypothesis of the reactor flux anomaly. The Spectral Deviation Daya Bay and other θ13 experiments observed bump in 4-6 MeV region, a deviation of ~10%. Physics Goal 2: To make a precise measurement of the antineutrino spectrum from a HEU reactor (mainly U235). New experiments need to be reactor model-independent APS/POPA Entries / 250 kev i Reactor Flux Anomaly Ratio to Prediction Entries / 250 kev (Huber + Mueller) Ratio χ 2 contribution to Prediction (Huber ( χ + ) Mueller) tion Data Full uncertainty Reactor uncertainty ILL+Vogel Data Full uncertainty Integrated Reactor uncertainty ILL+Vogel 2 Prompt Positron 4 Energy (MeV) 6 8 Daya Bay Integrated 2 Prompt 4Energy (MeV) Prompt Energy (MeV) Local p-value (1 MeV windows) lue ows)

22 Experimental site: High Flux Isotope Reactor exterior door reactor wall PROSPECT-20 shield Antineutrino Detector I Established on-site operation User facility, easy 24/7 access Exterior access at grade Full utility access, incl. internet HFIR core Supported by: APS/POPA

23 HEU to LEU and HFIR (redux) (with input from David Renfro and Tim Powers)

24 HFIR staff have worked closely with NNSA since 2005 to support LEU conversion 2006 Basic assumptions established 2011 Preliminary LEU design Alternate LEU design studies No changes to Physical dimensions Geometry Clad material Cycle length (~24-26 d) Margin of safety in SAR Coolant flow rate Subcriticality of elements Storage methods Analysis indicated reactor s ability to perform its scientific missions will not be diminished by conversion if: Power is increased from 85 to 100 MW Fuel region within the fuel plate is axially contoured (bottom 3 cm) Purpose Support NNSA s effort to qualify and manufacture (in a stable, repeatable manner) a robust, affordable LEU fuel Alter/optimize or eliminate complex features of the preliminary design which seem problematic for the manufacturing process Conversion must maintain HFIR mission APS/POPA

25 Complex LEU fuel design process Performance Requirements Performance Analysis HFIR LEU Fuel Design APS/POPA

26 Complex LEU fuel design process Performance Requirements Performance Analysis HFIR LEU Fuel Design Safety Analyses Regulatory Safety Criteria APS/POPA

27 Complex LEU fuel design process Performance Requirements Performance Analysis HFIR LEU Fuel Design Safety Analyses Regulatory Safety Criteria Manufacturing Flowsheet Cost APS/POPA

28 HFIR conversion planning continues HFIR conversion will occur in five phases Develop analytical tools and demonstrate feasibility of HFIR conversion (reference safety basis) Demonstrate operation of HFIR with HEU fuel at 100 MW Conduct low-power testing of LEU lead test core in vessel Conduct high-power testing of LEU lead test core in vessel with PIE Demonstrate operation of HFIR with production LEU fuel at 100 MW Based on preliminary performance and safety analyses conducted to date, ORNL believes that HFIR can be converted and maintain its world-class mission performance provided LEU fuel can be: Qualified to HFIR conditions Manufactured to HFIR specifications Demonstrated to be reliable and affordable APS/POPA

29 Questions? APS/POPA