ORNL is managed by UT-Battelle for the US Department of Energy

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

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Outline

• ORNL’s role in the DOE Isotope Program • HFIR and isotope applications • HEU to LEU and HFIR (redux) • Questions

ORNL’s role in the DOE Isotope Program

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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

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Facilities supporting DOE Isotope Program

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DOE Isotope Program funding and engagement Statutory Authority: Public Laws 101-101 (1990) and 103-316 (1995)

•  The annual appropriation in NP funds a payment into the revolving fund to –  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: –  Annual strategy meetings

–  Stakeholder meetings

–  Federal Workshop

–  DOE/NIH meetings

–  National Isotope Development Center

–  NSAC

Isotope Program Operations DOE/SC/NP

Community Engagement

Collections from isotope

sales

Annual Appropriations

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•  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

The ORNL Isotope Program Strategy

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.

•  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 Vision ORNL assets

HFIR and isotope applications

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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…

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High Flux Isotope Reactor Is a Unique Facility with Multiple Missions

Versatile 85 MW Reactor

•  Highest thermal flux in Western world •  2.5E15 n/cm2-s thermal •  1.2E15 n/cm2-s fast

•  Neutron Scattering Research •  Brightest cold neutron source in world

•  Isotope Production •  Material Irradiation •  Neutron Activation Analyses •  Neutrino R&D

Operations: SC/BES

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ORNL Radioisotopes

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HFIR produces diverse isotopes for a variety of applications

Energy Industrial Security Medical •  Nuclear fuel quality control •  Reactor start-up sources •  Coal analyzers •  Oil exploration

•  Mineral analyzers •  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

•  Cancer Treatments

Mars Rover Curiosity uses an RTG containing 3.6kg 238Pu to produce electricity. -NASA image

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Radioisotope production at ORNL •  252Cf •  63Ni •  75Se

•  225Ac •  212Pb •  188W •  227Ac

ORNL also dispenses high purity 242Pu, 234U, 239Pu, and

243Am from inventory

•  89Sr •  109Cd •  133Ba •  14C

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Example: Cf-252, many industrial and research apps

Fm

Es

Fm 254 Fm 255 Fm 256

SF

Fm 257

Es 254 Es 255

- EC -

CfCf 249

, (n,f)

Cf 250 Cf 251 Cf 253 Cf 254

, ,

, (n,f) ,

Bk 249Bk

Bk 250 Bk 251

-

Cm 242

Am

Cm

Pu 246

Cm 243

Pu 239

, (n,f)

, (n,f)

Cm 244 Cm 245

, (n,f)

Cm 246

, (n,f)

Cm 247

, SF

Cm 248

SF

Cm 249 Cm 250

Pu 240

Np 237

Pu 238 Pu 241 Pu 242 Pu 243

Np 238

Pu 244 Pu 245

-, (n,f)

, (n,f)-

Am 241

, EC-

Am 242 Am 243 Am 244 Am 245 Am 246

94

93

95

96

N

Z

98

97

100

99

SF

--

-

---

- - -Pu

Np

Es 253

Cf 252

, SF

•  Feedstock (heavy curium) in place for 15+ years

•  DOE produces at ORNL for a consortium

•  Variety of uses

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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=117 – 120

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Naming of element 117 Tennessine (Ts)

28th 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)

(and we are not done with new element discoveries)

Bk-249 targets produced at HFIR

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It takes time to develop isotopes: The story of 82Sr/82Rb

•  1954: 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 1989

•  82Rb PET has better diagnostic accuracy than 99mTc-SPECT especially in obese patients

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: 10.3389/fmed.2015.00065

“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).”

Accelerator example. Applies to reactor production as well…

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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

Elgqvist et al., Front. Oncol. 3, 324 (2013) 50-70 µm 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)

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Alpha therapy in practice: 223Ra

•  Xofigo (radium-223 dichloride, Bayer)- First FDA Approved Alpha Therapy Agent in 2013

•  Ra-223 (t1/2 = 11.43 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)

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Alpha emitters

Issues •  Short half lives (production) •  Associated chemistry (how to get into the body) •  Toxicity (bi products) •  …

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PROSPECT Motivations and Goals PROSPECT is a DOE (HEP)-funded multi-phase short-baseline reactor experiment that will be installed at the High Flux Isotope Reactor (HFIR).

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

Antineutrino flux observed vs model. (PRL116, 061801)

T.J. Langford - Yale University Date/Seminar4

Prompt Positron Energy (MeV)2 4 6 8

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Daya Bay

ReactorFluxAnomaly

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Experimental site: High Flux Isotope Reactor

•  Established on-site operation •  User facility, easy 24/7 access •  Exterior access at grade •  Full utility access, incl. internet

HFIR core

Antineutrino Detector I

exterior door reactor wall

PROSPECT-20 shield

Supported by:

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

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HFIR staff have worked closely with NNSA since 2005 to support LEU conversion

2006 Basic assumptions

established

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

2011 Preliminary LEU design

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)

2012 - 2017 Alternate LEU design studies

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

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Complex LEU fuel design process

PerformanceRequirements

PerformanceAnalysis

HFIRLEUFuel

Design

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Complex LEU fuel design process

PerformanceRequirements

PerformanceAnalysis

HFIRLEUFuel

DesignSafety

AnalysesRegulatory

SafetyCriteria

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Complex LEU fuel design process

PerformanceRequirements

PerformanceAnalysis

HFIRLEUFuel

DesignSafety

AnalysesRegulatory

SafetyCriteria

Cost

ManufacturingFlowsheet

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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

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Questions?