Design and test of an Accelerator Driven Neutron Activator at the Joint Research Centre of the European Commission

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Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 1 Design and test of an Accelerator Driven Neutron Activator at the Joint Research Centre of the European Commission K. Abbas, G. Cotogno, N. Gibson, U. Holzwarth and F. Simonelli Institute for Health and Consumer Protection, Joint Research Centre, European Commission, Ispra (VA), Italy S. Buono and L. Maciocco Advanced Accelerator Applications (AAA), St. Genis Pouilly, France R. Rocca European Organisation for Nuclear Research (CERN), France/Switzerland N. Burgio ENEA, Casaccia, Italy G. Mercurio ENEA, Ispra, Italy 18 th International Conference on Cyclotrons and their Applications 2007

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 2 Outline ARC concept and previous experiments Motivation the INBARCA project New design for an ARC neutron activator Installation and preliminary results Concluding remarks

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 3 Adiabatic Resonance Crossing (ARC) concept - ARC was introduced by C. Rubbia for transmutation and radioisotope production (by neutron capture) - The ARC method consists of moderating neutrons in lead - Pb has the lowest capture cross section in the fast neutron field - In Pb fast neutrons are moderated in small energy degradation steps therefore neutron capture in the epithermal range (resonance range) is enhanced

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 4 Use of ARC Concept for Transmutation or Radioisotope Production 1 - Fast neutrons are generated in a target bombarded with accelerated charged particles 2 - Then they are incrementally slowed by scattering with relatively little energy absorption in lead down to the resonance energy range of the material to be transmuted 3 - Finally, they are captured in the material to be transmuted (neutron captures take place)

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 5 Transmutation by Adiabatic Resonance Crossing (TARC) Experiment at CERN (1996-1999) 1 - Facility installed in the CERN PS proton beam line 2 - Neutrons produced by spallation with proton beam (2.5-3.5 GeV) 3 - Neutrons slowed down in Lead (3.3 m x 3.3 m x 3 m, ~ 334 tons) 4 - TARC Conclusions: - ARC can be used to transmute large amounts of 99 Tc or 129 I (long lived f. products) - ARC can be used as an alternative method (alternative to nuclear reactors) for radioisotope production for medical or other applications

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 6 ARC experiment at the Cyclotron of Louvain-La-Neuve (Belgium) 1 Aim: Feasibility study for industrial production of 99 Mo (generator of 99m Tc) and 125 I using the ARC concept in a cyclotron (University of Louvain) 2 Neutron generated by proton beam (65-75 MeV) bombarding Be target 3 Neutron slowing down in pure lead (1.6 m x 1.6 m x 1.63 m, 47 tons) 4 Conclusion: The results were very encouraging and seem to confirm that the ARC concept can be used for radioisotope production for nuclear medicine

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 7 Aim of the current project - partially funded by the EUREKA programme, project INBARCA - (Innovative Nanosphere Brachytherapy by Adiabatic Resonance Crossing with Accelerators) 1 Test of a new ARC design concept at low energy (Cyclotron) 2 Measurement of activation yields and validation of MC calculations 3 Activation of nanoparticles for Brachytherapy (Ho and Re) 4 Investigation of other potential uses (other radioisotopes, activation of nanoparticles for tracer studies, etc.)

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 8 List of radioisotopes used in brachytherapy (in black) and the ones proposed in this project (in red) Radioisotope Symbol T 1/2 (h) Decay mode Mean energy Current production method Main applications 125-Iodine 125 I 1425.6 e 35 kev Reactor Prostate cancer 103-Palladium 103 Pd 407.76 ec 21 kev Reactor & Accelerator Prostate cancer 90g-Yttrium 90g Y 64.104 b- 930 kev Reactor Live cancer 192g-Iridium 192g Ir 1771.92 b-(95.24%) b+(4.76%) 317 kev Reactor HDR brachytherapy 188g-Rhenium 188g Re 16.98 b- 2 MeV Reactor Bone cancer, rheumatoid arthritis, prostate 186g-Rhenium 186g Re 89.25 b- 1 MeV Reactor Bone cancer, rheumatoid arthritis, prostate 166-Holmium 166 Ho 26.80 b- 2 MeV Reactor Liver Tumour

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 9 New design for an ARC neutron activator GRAPHITE REFLECTOR IRRADIATION CAVITY PROTON BEAM WATER MODERATOR AND COOLING TARGET LEAD BUFFER

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 10 System design: calculations MCNPX, FLUKA and STAR-CD codes were used for designing the new ARC facility Components taken into account in the simulations: - Be target (quality, thickness, shape) - Proton irradiation (energy, charge, shape) - The cooling water of the Be target (shape, flow) - The lead buffer and Graphite reflector (quality, shape) - Irradiation channels (positions) The final design was optimised for maximum activation yield (with thermal and epithermal neutrons) of Ho and Re in the irradiation channels

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 11 JRC Cyclotron (Ispra, Italy) Scanditronix MC 40 RF cavities 2, lombda/4 Particles Minimum Energy (MeV) Maximum Energy (MeV) Maximum Extracted Current (ma) Dees Beam aperture 2, 90 degrees 20 mm p 8 40 60 Tuning Moving shorts/trim cap. a 8 40 30 3He2+ 8 53 30 d 4 20 60 RF range 12.5 27 MHz Frequency stability < 10-6 Amplitude stability < 10-3 Max. Dee peak voltage 44 kv Ion source Pole diameter Magnet weight Main coils Max. Curr. P.I.G. Type 115 cm 60 tons 850 A Sectors 3 Hill gap Valley gap Max. magnetic field Extraction radius 100 mm 180 mm 2.1 Tesla 50 cm Trim coils 8 Harmonic coils 84 sets

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 12 Installation of the neutron activator Beam line Neutron activator Be target Dimension: 60 cm x 60 cm x 60 cm Weight: ~ 600 kg 8 irradiation channels

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 13 Control system of the neutron activator

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 14 Preliminary Results Activation of foils of Mo and Au 100000 10000000 10000 99 Mo 1000000 100000 198g Au and 196g Au Counts 1000 100 Counts 10000 1000 100 10 10 1 0 400 800 1200 1600 2000 γ-ray energy (kev) 1 0 500 1000 1500 2000 -ray enrgy (kev) 98/100 Mo(n,g/2n) 99 Mo 197 Au(n,g) 198g Au 197 Au(n,2n) 196g Au

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 15 Preliminary Results Activation of foils of Re and Ho 1000000 100000 186g Re and 188g Re 1000000 100000 166g Ho 10000 10000 Counts 1000 100 Counts 1000 100 10 10 1 1 0 400 800 1200 1600 2000 0 500 1000 1500 2000 γ-ray energy (kev) γ-ray energy (kev) 185/187 Re(n,g/2n) 186g Re 165 Ho(n,g) 166g Ho 187 Re(n,g) 188g Re

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 16 Preliminary Results Summary Radioisotope T 1/2 Reaction Yield (MCNPX) Yield Measured (Ispra) Yield Measured (LLN) 198 Au 197 Au(n,g) 198 Au 553.83 196 Au 197 Au(n,2n) 196 Au 1.99 198g Au 2.69 d 197 Au(n,g) 198g Au 724.20 194.46 * (526.99 **) 196g Au 6.2 d 197 Au(n,2n) 196g Au 1.58 24g Na 14.96 h 27 Al(n,α) 24g Na 5.37 99 Mo 66 h 98/100 Mo(n,g/2n) 99 Mo 7.13 1.85 * (5.02 **) 166 Ho 165 Ho(n,γ) 166 Ho 1650.00 166g Ho 26.8 h 165 Ho(n,g) 166g Ho 2520.00 186 Re 185 Re(n,γ) 186 Re 693.00 188 Re 187 Re(n,γ) 188 Re 1150.00 186g Re 3.7 d 185/187 Re(n,g/2n) 186g Re 385.00 188g Re 0.71 d 187 Re(n,g) 188g Re 2100.00 *Yield corrected for proton energy bombardment, ** Yield for 65 MeV proton energy as published (LLN), Yield unit: kbq/(µa.h.g), Measured yield uncertainties: < 10%

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 17 Conclusions 1 - A new concept of an ARC neutron activator was designed and tested. With respect to previous designs it is much more compact (60 x 60 x 60 cm 3, weight ~ 600 kg) 2 - Preliminary results on activations of foils of various materials were in good agreement with calculations 3 - With reference to previous work, slightly higher production yields of 99 Mo (generator 99m Tc) and 198g Au were obtained (factor ~4) 4 - The promising activation yields accomplished in this work open interesting perspectives for brachytherapy studies using Ho and Re based radioactive nanoparticles 5 - The ARC activator developed in this work may constitute an attractive alternative to nuclear reactors for production of certain radioisotopes for medical or other applications

Giardini-Naxos, Italy, 30 September - 05 October 2007, Cyclotrons 2007 Conference 18 THANK YOU FOR YOUR ATTENTION