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2018-10-23

Medical Isotope Collection from ISAC Targets

PETER KUNZACCELERATOR DIVISION

INTDS Conference 2018

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2018-10-23

ARIEL -

Advanced Rare IsotopE

Laboratory

ISAC

2 proton beam target

stations (alternate

operation)

ARIEL (under construction)

1 e-beam target station

1 proton beam target station

(+ symbiotic target for

medical isotope production)

hot cell infrastructure for

processing of irradiated

targets

Radioactive Ion Beam Facilities at TRIUMF

Vancouver, BC

ISAC – ISOL Facility

3

500 MeV H- Cyclotron

100 μA

Ion Source

Target

Mass

Separator Mass-selected RIB to:

Experiments

Yield Station

Implantation Station

RIB

Geant4 Visualization Spallation

Fragmentation

Fission

Up to

50 kW beam power

Radioactive Ion Beams at ISAC

4

Radioactive Ion Beams at ISAC

http://mis.triumf.ca/science/planning/yield/beam

http://isys01.triumf.ca/search/yield/data (new)

• Nuclear structure and reactions

• Nuclear astrophysics, element formation

• Symmetry studies

• Material science

• Isotopes for medical research

ISAC Targets

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Target Properties

Example: Uranium carbide target

Reaction rate with proton beam 10-30 %

5000 μAh p+ irradiation results in ~0.00018 mol reaction products (>2000 isotopes)

Max. production quantities for individual isotopes 1-2 μmolEstimates based on GEANT4 Simulation

200 mm

Ø19mm

Composite Ceramic Uranium Carbide Targets

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• milling to <10µm particle size

• UC2/C slurry is poured on graphite foil

• Stacks of cut-out target disks are loaded into the

tantalum target container and sintered in-situ• average thickness per disc ~ 50 mg/cm2

• Density 3-3.5 g/cm3 (~ 30% theo. density)

• ~ 250 Discs per target

19 m

m

UO2 + 4C → UC2 + 2CO(g) Carbothermal reduction at 1750 °C

30 µm

• New, faster approach: carbothermal reduction on graphite foil in graphite target insert

Kunz, P. et. al., J.Nuc. Mat. 2013 Sep;440(1–3):110–6.

Cervantes, M. et al., IPAC2018, doi:10.18429/jacow-ipac2018-thpml131

ISAC Implantation station

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• Beam current monitoring during

implantation

• Collimators allow accurate beam

tuning and limit spread of

contamination by recoils

• Sample transfer to hotcell or

fumehood under vacuum

223,224,225Ra,225Ac209,211At, 165Tm/Er

http://srim.org/

Medical Isotopes from ISAC

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Isotope Half-life Application Production method Target

Ion

source

Measured

yield rate

Acuumulated activity (2

shifts = 86400s) [Bq] Activity [Ci]

225Ac 9.92 d TAT 225Ac implantation Uranium carbide LIS 1.30E+08 8.60E+06 2.32E-04

225Ac 9.92 d TAT 225Ra implantation/decay Uranium carbide SIS 1.70E+08 3.40E+06 9.19E-05

224Ra 3.66 d TAT 224Ra implantation Uranium carbide SIS 1.60E+09 2.70E+08 7.30E-03

223Ra 11.43 d TAT 223Ra implantation Thorium oxide SIS 6.90E+08 4.00E+07 1.08E-03

213Bi 45.6 m TAT 225Ac implantation/decay Uranium carbide SIS 6.70E+07 2.25E+06 6.08E-05

212Pb 10.64 h TAT 224Ra implantation/decay Uranium carbide SIS 1.60E+09 1.00E+08 2.70E-03

212Bi 60.6 m TAT

224Ra implantation/decay via

212Pb Uranium carbide SIS 1.60E+09 7.80E+07 2.11E-03

211At 7.22 h TAT 211Rn implantation/decay Uranium oxide FEBIAD 1.00E+08 2.40E+07 6.49E-04

211At 7.22 h TAT 211At implantation Uranium oxide FEBIAD 8.40E+07 7.40E+07 2.00E-03

211At 7.22 h TAT 211Fr implantation/decay Uranium carbide SIS 1.90E+09 4.30E+07 1.16E-03

209At 5.4 h SPECT Fr213 implantation Uranium carbide SIS 1.80E+09 8.50E+08 2.30E-02

209At 5.4 h SPECT At209 implantation Thorium oxide LIS 1.90E+08 1.70E+08 4.59E-03

177Lu 6.65 d beta therapy 177Lu implantation Tantalum LIS 6.50E+08 6.40E+07 1.73E-03

169Yb 32.02 d SPECT 169Yb implantation Tantalum LIS 5.10E+10 1.00E+09 2.70E-02

166Yb 2.36 d Auger therapy 166Yb implantation Tantalum LIS 1.50E+11 3.70E+10 1.00E+00

165Er 10.3 h Auger therapy 165Yb/165Tm implantation Tantalum LIS 9.32E+10 3.90E+10 1.05E+00

161Ho 2.5 h Auger therapy 161Ho implantation Tantalum LIS 9.96E+09 9.30E+09 2.51E-01

161Ho 2.5 h Auger therapy 161Er implantation/decay Tantalum LIS 1.03E+10 3.90E+09 1.05E-01

149Tb 4.12 h TAT/SPECT 149Tb implantation Tantalum SIS 5.78E+08 5.75E+08 1.55E-02

140Nd 3.37 d PET/Auger therapy 140Sm implantation/decay Tantalum LIS 9.70E+08 1.70E+08 4.59E-03

124I 4.18 d PET 124I implantation Uranium oxide FEBIAD 2.20E+08 3.20E+07 8.65E-04

123I 13.22 h PET 123I implantation Uranium oxide FEBIAD 3.80E+07 2.60E+07 7.03E-04

082Sr 1.35 d PET 82Sr implantation Niobium SIS 1.00E+10 2.10E+08 5.68E-03

077Br 57.0 h Labeling 77Rb implantation/decay Niobium SIS 1.60E+09 3.70E+08 1.00E-02

067Ga 78.28 h Imaging 67Ga implantation Zirconium carbide LIS 8.10E+09 1.50E+09 4.05E-02

067Cu 2.58 d beta therapy 67Cu implantation Tantalum LIS 1.40E+08 3.10E+07 8.38E-04

064Cu 12.70 h PET/therapy 64Cu implantation Niobium LIS 3.20E+09 2.20E+09 5.95E-02

061Cu 3.33 h PET 61Cu implantation Niobium LIS 7.80E+08 7.50E+08 2.03E-02

Retrieving Activity from Implantation Target

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Sample preparation:

- pick-up in 0.1N HCl

Add0.1 ml 0.1 N HCl

Evaporate

Add and

Retrieve0.1 ml 0.1N HCl

Evap.-Rinse Cycles

Resid

ual A

ctivity (

Bq)

Alpha Recoil Collection

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225

Ac Decay Chain – Recoil tracks

typical alpha recoil

energy

~100 keV

Geant4 recoil track

simulation

Al target

Vacuum

213Bi Recoil Collection

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Source

Catcher

225Ac

213Po217At221Fr

213Po

217At221Fr213Bi

Efficiency

• up to 50% in 50-200 mbar Ar

• ~ 35% in air

• ~25% into aqueous solution

(allows quick and simple

radiolabeling and chelation

studies with 213Bi and 212Pb)

Bias

>20V

-

+

225

Ac Imaging Studies

AKH Robertson et. al., Phys. Med. Biol. 62 4406 (2017)

isolated 213Bi

225Ac, 221Fr,213Bi

A. Robertson

Ac/Bi Imaging Studies

209/211

At theranostic system

211Att1/2= 7.2 h

209Att1/2= 5.4 h

TherapyImaging

(α-emitter)(γ-emitter)

Crawford

Ruth

(from 213Fr alpha decay) (from 211Fr β+ decay)

Crawford et.al.

Applied Radiation and Isotopes. 2017 Apr;122:222–8

Crawford et.al.

Nuclear Medicine and Biology. 2017 May;48:31–5

J. Crawford, T. Ruth

At Theranostic System

Summary

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Collection of Isotopes for pre-clinical nuclear medicine research at the ISAC

Implantation Station (IIS)

- At, Ra and Ac for targeted alpha therapy from uranium carbide targets

- Tm/Er for Auger Therapy from tantalum targets

Retrieval of implanted activity

- By etching

- By recoil collection

• Upgrade of IIS (shielding, remote handling) to allow higher activities (up

to 1 Ci for certain lanthanides).

• Expand number of isotopes that can be provided (Tb, Ho, Yb, Lu, …)

• Development of implantation targets (minimization of chelation inhibitors)

Outlook