Summary of NSAC-Isotope Subcommittee Report, 2015

Transcription

1 Summary of NSAC-Isotope Subcommittee Report, 2015 Meeting Isotope Needs and Capturing Opportunities for the Future: The 2015 Long Range Plan for the DOE-NP Isotope Program Saed Mirzadeh Low Energy Community Meeting, East Lansing, MI, August 21, 2015 ORNL is managed by UT-Battelle for the US Department of Energy

2 NSAC-I Subcommittee Kelly Beierschmitt, Idaho National Laboratory Roy Brown, MBA Mallinckrodt Pharmaceuticals Carol Burns, Los Alamos National Laboratory Lawrence Cardman, (chair) Thomas Jefferson National Accelerator Facility Donald Geesaman, (ex officio) Argonne National Laboratory Suzanne Lapi, Washington University, St. Louis Saed Mirzadeh, Oak Ridge National Laboratory Eugene Peterson, Los Alamos National Laboratory Lee Riedinger, University of Tennessee J. David Robertson, University of Missouri Thomas Ruth, TRIUMF David Scheinberg, Memorial Sloan Kettering Cancer Center Sally Schwarz, Washington University, St. Louis Bradley Sherrill, Michigan State University Mark Stoyer, Lawrence Livermore National Laboratory Scott Wilbur, University of Washington Frank Yeager, Eckert and Ziegler Isotope Products

3 The mission of the DOE Isotope Program: 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 that can make available new isotopes for research and applications.

4 Background The Isotope Program is a relatively small federal program: FY15 federal appropriation: $19.84 M FY15 anticipated isotope sales of ~$36 M This small programs, however, enables and is immersed in billion-dollar enterprises, including medical diagnosis and treatment, research, national security, and critical industries. These applications touch the lives of almost every citizen. 4 Isotope Program S&T Review

5 NSAC-I 2015 Report Contents Executive Summary Chapter 1: Introduction Chapter 2: The DOE Isotope Program Chapter 3: Uses of Isotopes Chapter 4: Research Opportunities Using Isotopes Chapter 5: The Scope and the Scientific/Technical Challenges for the Isotope Program Chapter 6: Sources of Isotopes for the Nation Chapter 7: Research and Development for Isotope Production Chapter 8: Trained Workforce and Education Chapter 9: Program Operations Chapter 10: Budget Scenarios References Appendices

6 Application Diagnostic imaging of human disease Therapy of human disease Fixed therapeutic sources Biological, biochemical, and chemical research tracers Power sources Nuclear and particle physics, chemistry and engineering Fission and reactor function Environment, security and safety Stable Isotopes Selected Isotope Examples Gamma imaging: 201 Tl, 99m Tc, 111 In, 131 I, 133 Xe Positron (PET) imaging: 18 F, 124 I, 68 Ga, 89 Zr, 64 Cu, 86 Y, 11 C, 15 0, 82 Sr/ 82 Rb Beta-emitters: 131 I, 90 Y, 89 Sr, 177 Lu, 186/188 Re, 153 Sm Alpha-emitters: 223 Ra, 225 Ac, 211 At, 213 Bi, 212 Pb/ 212 Bi External beams: 60 Co Internal brachytherapy: 192 Ir, 125 I 3 H, 32 P, 33 P, 125 I, 35 S, 51 Cr, 75 Se, 14 C 244 Cm, 238 Pu, 210 Po, 90 Sr, 237 Np, 239 Pu, 244 Pu, 243 Am, 248 Cm, 249 Bk, 249 Cf, 225 Ra, 48 Ca 233 U, 235 U, 238 Pu Sensors, tracers and detectors: 241 Am, 137 Cs, 252 Cf, 6 Li, 14 C, 3 He, 75 Se, 133 Cs, 65 Ni Coolants: 7 Li, 10 B 13 C, 15 N, 18 O, Many

7 The Network of DOE Isotope Production Sites and examples of isotopes produced or distributed from each site.

8 Recommendations significant increase of funding for Research and Development a) Continue support for R&D on the production of alpha-emitting radioisotopes. b) Support R&D into the production of high specific activity theranostic radioisotopes: 99m Tc/ 188 Re, 111 In/ 90 Y. c) Support for R&D on the use of electron accelerators for isotope production: 68 Zn(γ,p) 67 Cu, 232 Th(γ,spall) 225 Ac 232 Th(γ,spall) 211 Rn(t 1/2 =14.6 h, EC) 211 At. a) Support R&D on the development of irradiation materials for targets that will be exposed to extreme environments to take full advantage of the current suite of accelerator and reactor irradiation facilities b) Completion and the establishment of effective, full intensity operations of the stable isotope separation capability at ORNL

9 Recommendations (cont.) Increase in the annual appropriated budget for high-impact infrastructure investments and to maintain a stable funding base for reliably operating and continually improving facilities. a) Infrastructure for isotope harvesting at FRIB b) Develop a strategy for the re-establishment of a separator for radioactive isotopes to support research c) Increase the base infrastructure budget to sustain and expand production capacity at the Isotope Program facilities at BNL-BLIP and LANL-IPF Continuation and expansion of the effort to integrate the university facilities with the Isotope Program 9 Isotope Program S&T Review

10 Applications and Uses of Isotopes in Nuclear Physics Investigation of the structure and reactions of atomic nuclei The Argonne Tandem Linac Accelerator System (ATLAS) and Californium Rare Ion Breeder Upgrade (CARIBU); requiring 1 Ci 252 Cf source 1½ - 5 years National Superconducting Cyclotron Laboratory (NSCL); 48 Ca, 86 Kr, 82 Se, and others Rare Isotope Beams (FRIB); new opportunity to access a broad range of radioactive isotopes through isotope harvesting. Example include: a) Harvesting 48 V or 147 Eu- 154 Eu, and potential to provide increased quantities of 223 Ra and 225 Ra, and search for more sensitive candidates, such as 229 Pa. b) Providing beams of 16 C, 17 N, 20 O for synthesizing very long-lived isotopes of rutherfordium, dubnium, and seaborgium with projected t 1/2 > 1 y c) Measurement of cross-section of very short-lived radionuclides via inverse kinematics reactions

11 Nuclear Physics (cont.) Permanent electric dipole moment (EDM) of a quantum system Requiring multi mci of 225 Ra and 223 Ra as potential high-sensitivity deformed nuclei Neutrinoless Double Beta Decay: 76 Ge 76 Se 136 Xe 136 Ba, 130 Te 130 Xe, 48 Ca 48 Ti. Requiring a ton of active material

12 Nuclear Physics (cont.) Synthesize of Heaviest Elements using Actinide Targets Six heaviest elements, A= , was discovered using actinide targets of 237 Np, 239,240,242,244 Pu, 243 Am, 248 Cm, 249 Bk and 249 Cf target mainly produced in the U.S. In 2009, Element 117 was synthesized via 48 Ca Bk reaction by a 150-day irradiation of 22 mg of 249 Bk in Dubna at the U-400 cyclotron with 48 Ca beam 22 mg of chemically purified 249 Bk prior to shipment to Dmitrovgrad. Future targets are envisioned to require > 100 mg.

13 Planetary science Use of 238 U, 234 U, 230 Th, 232 Th and 226 Ra as geochronologic tools for study of magmatic differentiation or deposition of carbonate rocks; requiring very high purity 233 U and 229 Th (very low contamination from both 230 Th and 232 Th) as calibration standards of mass spectrometer Solid-state physics Avogadro s project on going project to develop a mass standard based on fundamental units; measuring the uncertainty of Avogadro constant to 0.01 ppm. Project requiring kilograms of isotopically pure 28 Si.

14 Radioisotopes for calibration of neutrino detectors 51 Cr, 144 Ce, freshly irradiated Cm targets, fresh HFIR spent fuel, etc. For example, preliminary calculations indicate that six fresh Cm targets arranged in a flux-trap configuration could provide the highest flux of man-made neutrinos. In the later three examples, the key challenge is that the magnitude and size of required radioisotopes require interagency agreements, and substantial funds.

15 Nuclear Data for Weapons Physics Research With the cessation of nuclear testing in 1992, it has become necessary to develop sophisticated simulations of weapons performance that incorporate many different simultaneous nuclear reactions taking place in the high neutron flux density environment. Simulations must be empirically validated by comparing the historic data from U.S. weapons tests against predicted values. This generates need for accurate nuclear data. Principal reactions are: (n,γ),(n,f),, (n,α), (n,2n) While cross-sections are well known for stable isotopes, there is lack of data for short-lived radionuclides, and for reaction leading to metastable radionuclides; σ( A Z[n,n'] Am Z) >> σ( (A-1) Z[n,γ] Am Z)

16 93 Zr 1.5E6 y Key reaction cross sections near A=95 But 95 Sr is short lived and thus a target can t be made (n,γ) 94 Zr (n,γ) 95 Zr (n,γ) 96 Zr (n,γ) 97 Zr (n,2n) Stable (n,2n) d (n,2n) Stable (n,2n) 16.8 h β β β β β (n,γ) (n,γ) Y Y 95 (n,γ) Y 96 (n,γ) Y 0.9s/10.2h (n,2n) 18.7 m (n,2n) 10.3 m (n,2n) 9.6s/5.3s (n,2n) β Known cross-sections 93 Sr 7.41 m β 93 Rb 5.85 s Measured 93 Kr 1.29 s 97 Y 1.2s/3.8s β β β β (n,γ) (n,γ) (n,γ) (n,γ) 94 Sr 95 Sr 96 Sr (n,2n) 1.25 m (n,2n) 25.1 s (n,2n) 1.07 s (n,2n) β 97 Sr 0.43 s β β β β (n,γ) 94 (n,γ) Rb 95 (n,γ) Rb 96 (n,γ) Rb (n,2n) 2.71 s (n,2n) 377 ms (n,2n) 199 ms (n,2n) Importance Factor IF = IY * ADT IY is maximum independent yield ADT = 2 (A=95), 1 (A=94,96), 0.5 (A=93,97) 97 Rb 169 ms β β β β (n,γ) 94 (n,γ) Kr 95 (n,γ) Kr 96 (n,γ) Kr (n,2n) 0.21 s (n,2n) 0.78 s (n,2n) UK (n,2n) 97 Kr <0.1 s IF > < 0.1 National Criticality Experiments Research Center (NCERC) located at the Nevada National Security Site provides access to relevant fission-spectrum irradiation capabilities. For very short-lived species, FRIB will provide the opportunity to examine in-beam reactions

17 Nuclear Data for Production of Actinium-225 Background of Ac-225 production ORNL has been the main supplier of 225 Ac (via decay of existing 229 Th stock) since 1997, mci of 225 Ac is harvested annually from 130 mci 229 Th stock at ORNL. 233 U α 1.6x10 5 y 229 Th α 7.9x10 3 y 225 Ra β 15 d 225 Ac 6-12 campaigns are performed per year, and campaign 120 is currently underway α 10 d Rationale for R&D related to production of Ac-225 The present supply of 225 Ac is insufficient for current medical and research demands of ~6 Ci/year. Ac-225 (mci) Annual Production of Ac Year Number of shipment Production Capacity Dispensed Amount Shipments xaaaaaaaaaaaa

18 New Initiatives to Enhance Production of Actinium-225 for Cancer Treatment The initiatives are a direct response to the NSAC-I recent citation on the gap between production and demand of this medically useful isotope Projects Time frame Comments Direct production of Ac-225 in a proton accelerator 2012-Cont. Target irradiation at BNL and LANL, processing at ORNL Nuclear Data for Reactor Production of 229 Th and 227 Ac at ORNL-HFIR Nuclear Data for Production of 229 Th via low energy protons at ORNL Tandem NP R&D Grant NP R&D Grant

19 Direct production of 225 Ac in a proton accelerator The new collaboration between ORNL, BNL and LANL aims at developing a plan for full-scale production and stable supply of 225 Ac by irradiating 232 Th targets in the BNL BLIP and LANL IPF 232 U 68.9 y 233 U 1.59E5 y 228 Pa 22 h 229 Pa 1.4 d α εc 227 Th 18.7 d 228 Th 1.91 y 229 Th 7340 y 230 Th 7.54E4 y 231 Th 25.5 h 232 Th 1.4E10 y 225 Ac 10.0 d 226 Ac 29.4 h 227 Ac 21.8 y 228 Ac 6.15 h? 229 Ac 1.05 h β 224 Ra 3.66 d n,γ 225 Ra 14.9 d 226 Ra 1600 y 227 Ra 42.2 m? 228 Ra 5.75 y? 229 Ra 4.0 m 19 Isotope Program S&T Review

20 Direct production of 225 Ac in a proton accelerator (cont.) BNL targets: 1-3 foils ~850 mg each. LANL : one 10-g target Irradiations: BLIP: µa at MeV, IPF: 200 µa of MeV Issues: Transportation: Rad Dose & Activity Limits Radiological Limits of Processing Facility Very Complex Chemistry Cross-Section (mb) This Work Weidner, 2012 Ac-225 Effective Cross Section Rather short half life of 225 Ac, and ~0.2% contamination with 227 Ac at EOB Energy (MeV) 20 Isotope Program S&T Review

21 Nuclear Data for Reactor production of Th-229 σ = 457 ± 195 b 21 Isotope Program S&T Review

22 Reactor Production of 227 Ac, 228 Th and 229 Th from 226 Ra Target HFIR Hydrualic Tube Irradiation Facility, φ n =1x10 15 n.s -1.cm Th Activity (mci/mg of 226 Ra) Ac-227 Th Irradiation Time (d) Projected 229 Th yield for 6 cycle irradiations: mci per g of 226 Ra, with 228 Th and 227 Ac contaminations of ~3000 and 50 times larger. 20 mci of 229 Th will generate ~140 mci of 225 Ac per year 22 Isotope Program S&T Review

23 Nuclear Data for Production of 229 Th via Proton-induced Reactions on 232 Th Pa d (p,2n) (p,4n) α (0.5%) ε (99.5%) Th y (p,d) (p,pn) Th y (p,nt) (p,2nd) (p,3np) Th y β Ac m (p,2p) β Ra m (p,α) (p,pt) (p,n 3 He) (p,2d) (p,npd) (p,2n2p) (p,p 3 He) (p,2pd) (p,3pn) 500 Various Excitation Functions for Proton Bombardment of 232 Th Thorium Proton Bombardment Reaction Block Diagram Th[p,3n] 230 Pa (Morgenstern, 2009) 232 Th[p,3n] 230 Pa Counts 1e+5 1e+4 γ-ray Spectrum of Purified Pa Fraction (Th230-2, PaPPT-T5, 6/15/2011) 93 kev X-rays of Th ( 228 Pa, 229 Pa & 230 Pa) 108 kev 140 kev, 99 Mo 129 kev, 228 Pa Cross Section (mb) Th[p,4n] 229 Pa 232 Th[p,x] 229 Th 232 Th[p,5n] 230 Pa 1e Th[p,n] 232 Pa 1e Channel Number xaaaaaaaaaaaa Energy (MeV)

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