High Energy Physics Division Seminar October 19, 2016

SERGEY CHEMERISOV

RADIOISOTOPE R&D AT ARGONNE’S LOW ENERGY ACCELERATOR FACILITY (LEAF)

OUTLINE

Upgraded linac facility description 3 MeV electron Van de Graaff Mo-99 production technology

development Fission of uranyl sulfate solution Gamma-n and n-gamma reaction

on Mo-100 and Mo-98 Future isotopes Cu-67 Sc-47

2

L-BAND ELECTRON ACCELERATOR

LINAC type: Electron L band No load energy 55 MeV

Steady State Mode

Pulse width: 0.6-6.5 µs Repetition rate: 1-240 p/s Peak current: 2.5 A Energy: 20-50 MeV

Transient Mode

Pulse width: 4, 6, 8, 10, 20 ns

Repetition rate: 1-240 p/s Peak current: 22 A

LINAC UPGRADE Beam parameters in Steady State Mode

Energy (MeV) 20 25 30 35 40 45 50 Beam Peak Current (mA) 860 720 580 440 280 140 10

Average Beam Current (µA) 1118 936 754 570 364 182 13

Average beam power on the target (kW) 22.4 23.4 22.6 20.0 14.5 8.2 0.6

VAN DE GRAAFF ACCELERATOR (VDG)

VDF K3 Type: pulsed or D.C. – 0.3 – 3.0 MeV

Pulsed electron mode 1. Peak pulse current: - continuous variable 10 mA - 2 Amp 2. Pulse length: - fixed pulse width system -- 5, 10, 25, 55 and 100 nsec - variable pulse width system -- 50 ns - 10 us (duty cycle limitation) 3. Pulse repetition rate 1 - 1000 pulses/sec 4. Beam size ~ 0.5 cm diameter 5. Pulse amplitude stability --±2%

D.C. Electron Mode: 1. Max Current: 80 uA 2. Beam size: ~ 1cm diameter

RADIATION STABILITY TESTING AT VDG Testing of radiation stability of process equipment

Radiation damage tests using the

VDG Effects of photon radiation on

HDPE bottles containing K2MoO4 in 6 M KOH

Zero to 6.5 MRad shown (up to twice calculated dose expected)

Testing of RadioGenix generator components

6

Establishing a Reliable U.S. Domestic 99Mo Supply Convert research reactors and isotope production facilities from the use of HEU to LEU

• US work on production of 99Mo is funded under DOE’s NNSA Material Management and Minimization (M3) Program and has two primary goals

• Assisting current producers to convert from using HEU to LEU for production of 99Mo

• Accelerating the establishment of a reliable supply of commercial non-HEU-based 99Mo in the United States

The most common radioisotope used in diagnosis is 99mTc (daughter of 99Mo), with some 30 million procedures per year, accounting for 80% of all nuclear medicine procedures worldwide.

Most of the world's supply of 99Mo comes from only five reactors, all of them 45 to 55 years old. The Canadian and Netherlands reactors required major repairs over 2009-10 and were out of action for some time, which created a global shortage of 99Mo

DEVELOPING A DOMESTIC SUPPLY OF 99MO

NNSA’s Material Management and Minimization Program (M3) has assisted or is currently assisting in the development of 6 different technologies for producing 99Mo Neutron activation of 98Mo

GE-Hitachi NorthStar Medical Technologies, LLC

Reactor irradiation of LEU targets GA Technologies

Accelerator γ/n Reaction on 100Mo NorthStar Medical Technologies, LLC

Solution-reactor production of fission-product 99Mo B&W technical Services group

Medical Isotope Production System (MIPS)

Accelerator-driven production of fission-product 99Mo SHINE Medical Technologies

All technologies assert they can produce 3000 6-day Ci/week (50% of US requirements)

Argonne had or currently has development activities in 4 of the 6 technologies

8

SHINE SUPPORT: ARGONNE MINI-SHINE EXPERIMENT

Argonne’s mini-SHINE experiment uses fissioning of 235U in a uranyl-sulfate solutions using photo-neutron target at Argonne electron linac to produce Mo-99, this experiment is designed to: Study the effects of fission on target-solution chemistry and radiolytic off-gas generation Demonstrate the recovery and purification of Mo-99 from an irradiated target solution Produce Mo-99 to ship to potential Tc-99m generator manufacturer partners

Phase 1 (completed January 2016 ) The linac was operated at 35 MeV and 10 kW beam power on the Ta target 5 L solution (140 g-U/L) were irradiated with neutrons generated through gamma-n

reaction in the tantalum target Maximum solution fission power density was ≤ 0.05 kW/L Up to 2 Ci of Mo-99 was produced per run

Phase 2 Experiment will be conducted at 35 MeV beam energy and up to 20 kW beam power 20 L solution will be irradiated with neutrons generated in a depleted-uranium (DU) target

(Zr clad DU disks were manufactured at LANL) Maximum solution fission power will be ≤ 0.5 kW/L Up to 20 Ci of Mo-99 will be produced

MINI-SHINE PHASE 2 EXPERIMENT (FLOW DIAGRAM)

Shielded Enclosure with Target Solution

Recirculating pump

Shielded Storage Tank

Gas Collection System

Separation Glove Box

Gas Analysis enclosure

e beam

Mo-99 Product Transfer

Cask

HEPA, Silver Zeolite Filters

He

Gas LinesLiquid Lines

General configuration of Phase 2 mini-SHINE experiment stays the same as Phase 1 experiment

Single shielded separation glove box replaces two glove boxes used in Phase 1

Relocation of equipment based on lessons learned from Phase 1

ARGONNE’S ROLE IN ACCELERATING DOMESTIC PRODUCTION OF MO-99 Major tasks

Preparation and irradiation of the uranyl-sulfate target solution

Development and design of the Mo-recovery system

Use of the LEU-Modified Cintichem process for Mo purification

Develop method for periodic cleanup of irradiated target solution

Radiation stability of system components

Developing an understanding of radiolysis effects on Solution chemistry Gas generation Precipitation

11

MO-99 PRODUCTION FLOW DIAGRAM

12

5 L SOLUTION IRRADIATION VESSEL

5L uranyl nitrate/sulfate solution in a SS 304 vessel Large access port for gas analysis, flow loop, thermocouple, neutron- flux monitor, etc. 15-cm light-water reflector/cooler Ta photo-neutron target

Mo-99 PRODUCTION VIA SHINE METHOD. PHASE 1.

Irradiation Power Current Time (hr) Energy

Mo-99 produced (mCi)

Met Purity Specs

Overall Mo-99 Yield

1 7.3 kW 208 µA 2 35 MeV 70 Yes 95%

2 9 kW 276 µA 8 35 MeV 350 Yes 86%

3 9.4 kW 269 µA 32 35 MeV 810 No 94%

4 9.8 kW 267 µA 20 37 MeV 380 Yes 42%

5 10 kW 270 µA 4 35MeV 520 Yes 85%

6 10 kW 270 µA 16 35 MeV 1500 Yes >90%

0

500

1000

1500

2000

2500

3000

3500

4000

0 5 10 15 20 25 30 35 40 45

Mo9

9 EO

B Ac

tivity

[mCi

]

Irradiation Time [h]

MCNPX Theoretical Production Curves

5 kW

6 kW

7 kW

8 kW

9 kW

10 kW

Ratio (X/99Mo) Product

Specification 131I/99Mo ≤ 5×10-5

103Ru/99Mo ≤ 5×10-5 132Te/99Mo ≤ 5×10-5

89Sr & 90Sr/99Mo ≤ 6×10-7 Σα/99Mo ≤ 1×10-9 Σγ/99Mo ≤ 1×10-4

EFFECT OF ELECTRON ENERGY AND VOLUME OF THE SOLUTION ON PEAK FISSION POWER

Dependence of the peak power in solution at 30 MeV electron energy on volume of the solution

Dependence of photoneutron yields normalized per kW of beam power for Ta and DU targets on electron beam energy simulated with MCNPX

PHASE 2 MINI-SHINE IRRADIATION SETUP

16

20L Tank

DU Target

Target Cask

Shielded Box

Beam Line

Bean Line Vacuum Tube Extension

Weld Connection DU Target

Cooling Line Connection Tube

DU TARGET DESIGN

Target Disk Thick Target Disk Thin

Spacer Thin Spacer Thick

Beam Window

Coolant Flow Across Disk Face

Flow Control Orifices

Support Bar and Flow Divider

Compression Spring Housings and Flow Divider

Disk Installed in Spacer

Coolant Outlet

OVERVIEW OF 20 L PROCESS TANK DESIGN

Inner Process Tank

Outer Cooling/ Moderator Tank

Target Sleeve Thru both Tanks

Instrument and Dry Well Penetrations

Connections for Top Cooling Coil and Condenser/Heat Exchanger and Process

Heat Exchanger/ Condenser Inside of Tank

Overall Tank Assembly Size: ø22” x 22” H

Removable Flange

View Port

Process Fluid Level

SUPPORT FOR NORTHSTAR MEDICAL RADIOISOTOPES

Major challenges Efficient delivery of high

power electron beam to the target

Stability of the beam position on the target

High power beam tune-up and diagnostic

Cooling of high power density target

Mo100γ Mo99gamma

neutron

Accelerator production

Motor

Blower

Mass Flow Meter

Filter

Pressure Vessel Heat

Exchangers

Target

PROCESSING OF IRRADIATED MO TARGETS

Long Term Solution – Photon Capture NorthStar’s linac methodology (γ,n)Mo-100

Patent pending for the recovery process

Dissolution apparatus

MO-99 PRODUCTION VIA GAMMA-N ON MO-100

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Irradiation date

100Mo-Enrichement (position) 99Mo in 6 disks, Ci Power Current

Time, hrs. Energy

1-21-15 99% (1-6) 0.92 4 kW 95 µA 19 42 MeV

3-19-15 97.4% (3-8) 2.9 7.56 kW 180 µA 21 42 MeV

3-26-15 95.1% (3-8) 2.2 7.56 kW 180 µA 19 42 MeV

5-7-15 99% (3-8) 4.2 9 kW 288 µA 24 35 MeV

9-17-15 99% (3-8) 12.4 9 kW 288 µA 6 days 42 MeV

1

10

100

1000

0 5 10 15 20 25 30

Mo-

99, m

Ci

disk position

MCNPX

experimental100Mo enriched 922 mCi Natural Mo

~300 mCi

1-21-15 Irradiation

BEAM LINE CONFIGURATIONS FOR ACCELERATOR BASED PRODUCTION FACILITY

Beam line elements: 1-linac, 2-fast acting gate valve, 3-quad magnets, 4-bending magnets, 5-OTR and IR cameras, 6-Beam stop, 7-non-linear beam optics, 8-beam position monitors, 9-collimator, 10-target, 11-gate valve vacuum sensor, 12-rastering magnet, 13-270o magnet

HIGH POWER BEAM STOP AND COLLIMATOR

23

High power beam stop

Power deposition from 42 MeV electron beam in aluminum

MATERIALS SELECTION FOR HIGH POWER TARGET

Material

Density (Kg/m3)

Thermal Conductivity

(W/m-°C)

Maximum Stress (MPa)

Minimum Window

Thickness (mm)

Maximum Temperature

(°C)

Figure of Merit (FOM)

INCONEL 718 8,221 17.3 456 1.15 403 1 Hastelloy X 8,221 26.0 *Disqualified

INCONEL 706 8,055 22.5 75 2.87 1,280 2.45 Waspaloy 8,193 17.3 357 1.30 481 1.13 Rene 41 8,249 17.3 507 1.09 388 0.96

L-605 Haynes Alloy 25

9,134 19.0 *Disqualified

316 SS 7,806 22.5 *Disqualified 250 Maraging

Steel 7,916 29.4 706 0.93 269 0.78

AerMet 100 7,889 31.2 793 0.87 249 0.73 2024-T81

Aluminum. 2,768 173.1 *Disqualified

6061-T6 Aluminum.

2,713 173.1 *Disqualified

Titanium alloy AMS 4910

4,484 13.9 175 1.88 497 0.90

Beryllium Standard grade

1,855 138.5 147 1.96 131 0.39

Magnesium alloy 1,800 77.0 *Disqualified

𝐹𝐹𝐹 =𝜌𝜌𝜌𝐼𝜌𝐼

ρ = density of material to be evaluated t = minimum acceptable thickness of material to be evaluated ρI = density of INCONEL 718 tI = minimum acceptable thickness of INCONEL 718 FOM = Factor of Merit

FINAL MATERIAL CANDIDATES FOR TARGET WINDOW

Inconel 718 Maraging Steel Beryllium

Stress due to pressure loading plotted as stress intensity in MPa

Results of the thermal modeling are shown here as plots of temperature (°C)

Material Maximum Beam Power (kW) Inconel 718 18 Beryllium 40

250 Maraging Steel 39

COPPER-67 68Zn(γ,p)67Cu

Distributed production “Clean” production with enriched

target (68Zn – 19%) Demonstrated with large targets Separation method: sublimation

Has been demonstrated with large targets

No dissolution of main zinc mass

Still requires dissolution and ion exchange step

Requires a high energy Linac 67Cu reaction has a threshold at ~15

MeV and a peak at ~26 MeV Enriched targets will virtually eliminate co-produced isotopes

Simplifies separation chemistry Exception is 67Zn, which is stable

0.00

2.00

4.00

6.00

8.00

10.00

12.00

0 10 20 30 40 50 60 70 80

Cro

ss-S

ectio

n (m

b)

Energy (MeV)

Cross-Section for the production of Cu-67 from Zn-68 via 68Zn(γ,p)67Cu

OVERVIEW OF TARGET STATION INSTALLATION

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Target Station

Transport Cart

TARGET STATION CROSS SECTION

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Lead Shielding Blocks Typ.

Target Station Converter

Beam

Target Removal Mechanism

Gripper

TARGET STATION CROSS SECTION

29

Crucible

Zinc Target

Side Flow Channels Top and Bottom

Graphite Seal

Back Al Cap

Threaded SST Plug

Exit Window

Front Flow Channel

O-ring Seals

0.33mm Converter Plates

Beam

Converter Housing

Target Station Housing

Converter Plate Support

Converter Plate Spacer

SCANDIUM-47 Similar to 67Cu production

Bremsstrahlung: 48Ti(γ,p)47Sc “Clean” production with enriched target

(48Ti – 73.7%) Requires a high energy Linac 47Sc reaction has a threshold at ~15 MeV

and a peak at ~22 MeV Enriched targets will virtually eliminate co-

produced isotopes

30

02468

10121416

0 10 20 30 40 50 60 70 80

Cros

s Sec

tion

(mb)

Energy (MeV)

Cross-Section for the production of 47Sc from 48Ti via 48Ti(g,p)47Sc

200 400 600 800 1000 1200 1400 1600

keV

47Sc

44Sc / 45Ti (511 keV)

46Sc

46Sc 48Sc 48Sc

44Sc

48Sc

CURRENT ISOTOPE DEVELOPMENT SHINE – 99Mo

-Produced and purified Mo-99 from sub-critical fission on UO2SO4

Mo-99 met purity specifications

-Developed separation methods >95% recovery on initial

recovery column >95% recovery on

concentration column >85% recovery from LEU-

modified Cintichem processing

-Developed specialized equipment for remote processing

Gas analysis Separations Full system monitoring Hot Cell operations

-Studied radiation effects Bubble formation Uranyl peroxide formation Mo-ABO stability

-Shipped Mo-99 to GE Healthcare for testing -Moving on to Phase II

NorthStar – 99Mo -Produced Mo-99 from solid targets

• Meets purity specs -Developed processing of targets

• Dissolution of Mo metal • Conversion to molybdate

-Optimization of large-scale dissolution conditions -Recycle process to recover >95% pure and valuable enriched 98Mo and 100Mo

• Precipitation route • Solvent extraction route

-Radiation stability studies at VDG • Generator system

components -PAT study for the Dispensing unit -Shipped Mo-99 to NorthStar for generator trials

67Cu -Cu-67 was produced with specific activity of 100 mCi/mg (67Cu/Cu) for 2-4 mCi -Separation of 2-4 mCi of 67Cu within 60 hours of irradiation with a high radiological purity -Main separation removes >99% of target material -Sublimation of ~100 g of irradiated zinc metal using alumina tube sublimation apparatus -Standardization of sublimation step is under investigation

-Demonstrated >99% recovery of metallic zinc from sublimation apparatus

• Vital for economical use of enriched targets

-Manipulator-friendly apparati are designed and being tested -ONP funding to develop production and distribution of 67Cu

47Sc -47Sc was produced from Ti foils and TiO2 solid targets -Proof-of-principal separations have been performed -47Sc isolated with a high radiological and chemical purity -Processing time >2 hrs

• Mo-99 work supported by the U.S. Department of Energy, National Nuclear Security Administration's (NNSA's) Office of Defense Nuclear Nonproliferation, under Contract DE-AC02-06CH11357.

• Cu-67 work was supported by the U.S. Department of Energy’s Office of Science, Office of Nuclear Physics – Isotope Development and Production for Research and Applications (IDPRA) and through a Cooperative Research And Development Agreement (CRADA) with Iotron Industries USA.

• Sc-47 work was supported by LDRD

• 47Sc • M. Alex Brown • Jerry Nolen • Sergey Chemerisov • John Greene • Roman Gromov • Megan Bennett • Holly Dinkel • George Vandergrift

• 67Cu • Dave Ehst • Del Bowers • Nick Smith • Sergey Chemerisov • M. Alex Brown • Roman Gromov • Jim Grudzinski • George Vandergrift • Jerry Nolen • Jim Bailey

• 99Mo • George Vandergrift • Sergey Chemerisov • Mark Williamson • Mandy Youker • Peter Tkac • John Krebs • Mike Kalensky • Jim Grudzinski • Art Gelis • Alex Brown • Andy Hebden • Thad Heltemes • Dominque Stepinski • Jim Byrnes • Jim Jerden • Bill Ebert • Candido Pereira • Marty Steindler • Del Bowers • Roman Gromov • Chuck Jonah • Vakho Makarashvili • Brad Micklich • Lohman Hafenrichter • Kurt Alford • Ken Wesolowski • Kevin Quigley • Jim Bailey • Del Bowers • Jackie Copple • Momen Abdul

ACKNOWLEDGEMENTS