No description available.

Zugl.: Stuttgart, Univ., Diss., 2007

Zugl.: Aachen, Techn. Hochsch., Diss., 2009

Zugl.: Karlsruhe, Univ., Diss., 2009

Introduction The Los Alamos Isotope Production Program commonly irradiates target stacks consisting of high, medium and low-energy targets in the “A-”, “B-”, and “C-slots”, respectively, with a 100MeV proton beam. The Program has recently considered the production of 57Co (t1/2 = 271.74 d, 100% EC) from 58Ni using the low-energy posi-tion of the Isotope Production Facility, down-stream of two RbCl salt targets. Initial MCNPX/ CINDER’90 studies predicted 57Co radioisotopic purities >90% depending on time allotted for decay. But these studies do not account for broadening of the proton beam’s energy distribution caused by density changes in molten, potentially boiling RbCl targets upstream of the 58Ni (see e.g., [1]). During a typical production with 230 µA average proton intensity, the RbCl targets’ temperature is expected to produce beam energy changes of several MeV and commensurate effects on the yield and purity of any radioisotope irradiated in the low-energy posi-tion of the target stack. An experiment was designed to investigate both the potential for 57Co’s large-scale production and the 2-dimensional proton beam energy distribution. Material and Methods Two aluminum targets holders were fabricated to each contain 31 58Ni discs (99.48%, Isoflex, CA), 4.76 mm (Φ) x 0.127 mm (thickness). Each foil was indexed with a unique cut pattern by EDM with a 0.254 mm brass wire to allow their position in the target to be tracked through hot cell disassembly and assay (see FIG. 1). Brass residue from EDM was removed with HNO3/HCl solution. The holders’ front windows were 2.87 and 1.37 mm thick, corresponding to predicted average incident energies of 17.9 and 24.8 MeV on the Ni [2]. Each target was irradiated with protons for 1 h with an average beam current of 218 ± 3 µA to ensure an upstream RbCl target temperature and density that would mimic routine production. Following irradiation, targets were disassembled and each disc was assayed by HPGe γ-spectroscopy. Residuals 56Co (t1/2 = 77.2 d, 100% EC) and 57Co have inversely varying measured nuclear formation cross sections between approximately 15 and 40 MeV. Results and Conclusion Distributions of 56,57,58,60Co were tracked as described in both irradiated targets. The distribution of activities matched expectations, with radioisotopes produced by proton interactions with the 58Ni target (56Co and 57Co) concentrated in the area struck by IPF’s rastered, annulus-shaped proton beam, and the distribution of radioisotopes produced by neutron-induced reactions (58Co and 60Co) relatively uniform across all irradiated foils. The potential range of such temperature variations predicted by thermal modeling (approx. ± 200 °C) corre-sponds to a density variation of nearly 0.2 g.cm−3, and a change in the average energy of protons incident on the low-energy “C-slot” of approximately 5 MeV, well-matched to the indi-rectly measured energy variation plotted in FIG. 3. No energy distribution in the plane per-pendicular to the beam axis has previously been assumed in the design of IPF targets. The effective incident energy measured by yields of 57Co and 56Co is, however, almost 5 MeV higher than those predicted using Anderson and Ziegler’s well-known formalism [2]. This discrepancy is supported by previous reports [3] and likely exacerbated compared to these reports by the large magnitude of energy degradation (from 100 MeV down to 30 MeV) in the IPF target stack. For more detailed discussion, refer to Marus et al.’s abstract, also reported at this meeting. While the experiments reported do confirm the potential for many Ci-scale yields of 57Co from months-long irradiations at the IPF, the level radioisotopic impurities 56Co and 58Co are concerning. Commercial radioisotope producers using U-150 (23 MeV) and RIC-14 (14 MeV) cyclotrons in Obninsk, Russia specify 56/58Co activities at levels <0.2% of available 57Co

Strontium-82 (t1/2 = 25.5 d) is one of the medical isotopes produced on a large scale at the Isotope Production Facility (IPF) of the Los Alamos National Laboratory (LANL), employing a high intensity 100 MeV proton beam and RbCl targets. A constant increase in the 82Sr demand over the last decade combined with an established thermal limit of molten RbCl salt targets [1,2] has challenged the IPF’s world leading production capacity in recent years and necessitated the consideration of low-melting point (39.3 °C) Rb metal targets. Metal targets are used at other facilities [3–5] and offer obvious production rate advantages due to a higher relative density of Rb target atoms and a higher expected thermal performance of molten metal. One major disadvantage is the known violent reaction of molten Rb with cooling water and the potential for facility damage following a catastrophic target failure. This represents a significant risk, given the high beam intensities used routinely at IPF. In order to assess this risk, a target failure experiment was conducted at the LANL firing site using a mockup target station. Subsequent fabrication, irradiation and processing of two prototype targets showed a target thermal performance consistent with thermal modeling predictions and yields in agreement with predictions based on IAEA recommended cross sections [6]. Target failure test: The target failure test bed (FIG. 1) was constructed to represent a near replica of the IPF target station, incorporating its most important features. One of the most vulnerable components in the assembly is the Inconel beam window (FIG. 2) which forms the only barrier between the target cooling water and the beam line vacuum. The test bed also mimicked relevant IPF operational parameters seeking to simulate the target environment during irradiation, such as typical cooling water flow velocities around the target surfaces. While the aggressive thermal effects of the beam heating could not be simulated directly, heated cooling water (45 °C) ensured that the rubidium target material remained molten during the failure test. A worst case catastrophic target failure event was initiated by uncovering an oversized predrilled pinhole (1 mm Φ) to abruptly expose the molten target material to fast flowing cooling water. Prototype target irradiations: Two prototype Rb metal target containers were fabricated by machining Inconel 625 parts and by EB welding. The target containers were filled with molten Rb metal under an inert argon atmosphere. Follow-ing appropriate QA inspections, the prototype targets were irradiated in the medium energy slot of a standard IPF target stack using beam currents up to 230 µA. After irradiation the targets were transported to the LANL hot cell facili-ty for processing and for 82Sr yield verification. During the target failure test, cooling water conductivity and pressure excursions in the target chamber were continuously monitored and recorded at a rate of 1 kHz. Video footage taken of the beam window and the pinhole area combined with the recorded data indicated an aggressive reaction between the Rb metal and the cooling water, but did not reveal a violent explosion that could seriously damage the beam window. These observations, together with thermal model predictions, provided the necessary confidence to fabricate and fill prototype targets for irradiation at production-scale beam currents. X-ray imaging of filled targets (FIG. 3) shows a need for tighter control over the target fill level. One prototype target was first subjected to lower intensity (< 150 µA) beams before the second was irradiated at production level (230 µA) beams. During irradiation, monitoring of cooling water conductivity indicated no container breach or leak and, as anticipated given the model predictions, the post irradiation target inspection showed no sign of imminent thermal failure (see FIG. 4). Subsequent chemical processing of the targets followed an established procedure that was slightly modified to accommodate the larger target mass. TABLE 1 shows that post chemistry 82Sr yields agree to within 2 % of the in-target production rates expected on the basis of IAEA recommended cross sections. The table also compares 82Sr yields from the Rb metal targets against yields routinely obtained from RbCl targets, showing an increase in yield of almost 50 %.

Introduction The embrace of PET by medical clinicians has been reluctant (ΔT ≈ 20 yr) primarily due to the scale of the infrastructure that is needed. The capital cost of a cyclotron (≈ 106 USD) is now dwarfed by the demand for compliance to recent regulatory standards. This is a recurring expense, not only imposing an order-of-magnitude increase in staffing and operating costs, but damping the enthusiasm of researchers recalling the brisk pace of research in earlier days. Now an academic site, with little interest or opportunity to scale up production for wider distribution, is burdened by the new regulatory terrain of good manufacturing practice (GMP), mandated for translational studies that will reach only a few subjects. With our production resources held within a basic science department, the Medical Physics cyclotron facility at the University of Wisconsin has sought a sustainable pathway. We now anchor the operating budget by providing high-value, long-lived radionuclides to off-site users, to buffer the fluctuations of local demand for conventional PET synthons. Material and Methods: The tools of the trade The radioisotopes discussed here belong to the 3-d and 4-d sub shell, but are now moving into the rare-earths, with applications ranging from - targeted molecular imaging agents, - internal radionuclide therapy using to Auger electron-emitters, - to basic physics experiments using 163Ho (t1/2 ≈ 4500 yr) to determine the mass of the neutrino. Rather than focusing on the dozens of radionuclides produced, a number of tools deserve mention, as they support a variety of targets, reactions and products. These will be listed in order (A-G) from cyclotron to extraction to analysis. A. Two cyclotrons are used, a legacy RDS 112 (#1; 1985) and a GE PETtrace (2009). Neutron and gamma detectors are monitored during the long irradia-tions, signaling any subtle changes in the running conditions. (1). The PET-trace is fitted with a quick-change variable degrader target (2), as well as a beam-line with a 5-port (0 o, ±15 o, ±30 o) vertical switching magnet (3). The downward directed beam ports provide support for solid targets (e.g. Ga, S, Se, Te) that melt at low temperature. The irradiation of gas targets employs a generalized manifold to handle inert gases such as 36Ar for the production of 34mCl, as well as natural Kr and Xe for making Rb and Cs isotopes to act as fission product surrogates. These products are captured on a stainless steel target chamber liner, and rinsed off with warm water. The alkali metals are convenient tracers to study the ion exchange trapping process, pivotal in future 99Mo production from solution reactors (4). B. The preparation of malleable solid targets employs a 10-ton hydraulic bench press, and a jeweler’s mill to roll out foils from pellets, pressed between Nb foils to avoid contamination. C. Binary alloys are smelted in a programmable 1600o tube furnace under argon flow (eg. NiGa4). Alternatively, an induction furnace now permits highly localized heating of the binary metal charge, while allowing mechanical agitation during the smelting process. D. Electroplating onto gold discs is used for various enriched target material or the alloys above where quantitative recovery is essential, or where heat transfer from high beam current is demanding. E. The separation chemistry, prior to che-lation to targeted molecular imaging agents, is performed in LabView-driven, home-built “black boxes” resident in mini-cells (Radiation Shielding Inc.). F. Analysis of the targets after irradiation makes use of HPGe spectroscopy for gammas and characteristic X-rays of decay (e.g. rare earths). The elemental constitution of target alloys is deter-mined prior to irradiation by X-ray fluorescence analysis, excited by 109Cd and 241Am sources. G. Finally, broad-band elemental analysis at the ppb level now makes use of a microwave plasma atomic emission spectrometer (Agilent 4200), to be de-scribed elsewhere in this meeting. Results and Conclusions The tools above (A-G) are employed in the pro-duction of the expanded list of radionuclides offered by our cyclotron group to both local and off-site colleagues. The list below is ordered in terms of decreasing use, from regular production for national distribution (64Cu, 89Zr), to weekly inhouse use (44Sc, 66,68Ga, 68,69,71Ge, 72As, 61Cu, 86Y), to infrequent production for multi-site collaborations (163Ho, 95mTc, 206Bi): Radionuclide Target Employs 64Cu 64Ni/Au A, D, G 89Zr natY A, E, G 44Sc natCa A, B, E, F, G 66, 68Ga Zn/Ag A, B, D, E, F, G 68, 69, 71Ge Ga, GaO2 A, B, C, E,F 72As GeO2 A, B, E, F 52Mn natCr A, E, F, G 76, 81mBr SeO A, E, F 34mCl, Rb, Cs noble gas A, E, F 95mTc,163Ho Mo, Dy A, E, F TABLE 1. Target materials and processes. The production of long-lived radionuclides lends itself to crowd-sourcing, with distributed irradia-tion at virtually any site with a suitable accelera-tor and a relaxed beam schedule. A number of unique challenges do arise that don’t appear in the usual production of conventional cyclotron products such as 11C or 18F. Contamination by stable metals, inadvertently introduced by target pressing or beam-induced sputtering from degraders, can cause serious interference downstream limiting effective specific activity. Long-lived manganese isotopes are ubiquitous. And some very high value products are simply not within the reach of small cyclotrons, such as 52Fe and 67Cu, being too far off the line of beta stability. In conclusion, the research leading to a doctoral degree necessarily must focus on the physics and chemistry of novel radionuclides and tracers. On the other hand, clinical and translational research needs established imaging agents, with little room for innovation within the regulatory constraints. Our experience at Wisconsin has led us to a balancing act, with our routine production of clinical doses countered with our research program to provide high-value radionu-clides for our collaborative work with our basic science colleagues.

Zugl.: Wuppertal, Univ., Diss., 2006

Zugl.: Dortmund, Universiẗat, Diss.

Techn. Hochsch., Diss.--Aachen, 2007.