Qucosa – Hemholtz-Zentrum Dresden-Rossendorf
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Post irradiation evaluation of inconel alloy 718 beam window
Full text linkIntroduction
Annealed Inconel 718 alloy was chosen for the beam window at the Los Alamos Neutron Science Center (LANSCE) Isotope Production Facility (IPF) [1]. The window was replaced after 5 years of operation. Mechanical properties and microstructure changes were measured to assess its expected lifetime.
Material and Methods
A cutting plan was developed based on the IPF rasterred beam profile (FIG. 1). 3-mm OD samples were cut out from the window and thinned to 0.25-mm thick. Shear punch tests were per-formed at 25 °C on 21 samples to quantify shear yield, ultimate shear stress, and ductility. From 1-mm OD, 0.25-mm thick shear punched out disks, 4 TEM specimens of ~30×10×2 μm were obtained using standard FIB lift-out techniques. TEM was performed on an FEI Tecnai TF30-FEG operating at 300 kV.
Results and Conclusions
TABLE 1 shows MCNPX tally results of accumulated dpa, He and H content from both protons and neutrons fluences and ANSYS steady-state irradiation temperature for the 3-mm OD samples [2]. These peak values are at the peak density of Typically increases in shear yield and shear maximum stress occur with increasing dose. In this case, highest shear yield and ultimate stress was on the lowest dose samples at the outer edge (FIG. 2).
Optical microscopy images of the fracture surfaces on the shear punched out disks show no significant change in the fracture mode or reduction in ductility in the un-irradiated, high and low dose irradiated samples.
One un-irradiated and 4 irradiated samples (5, E, 16 and 19) were selected for TEM analysis. Figure 3 shows bright field TEM images of an un-irradiated, high and low dose irradiated samples.
Un-irradiated sample shows some dislocations and some large precipitates. The high dose sample #5 (~11 dpa, 122 oC) shows small loops and dislocations (left and center images) and no γ\' or γ\'\' precipitates in SAD from z = [011] (right image). Low dose sample #19 (~0.7 dpa, 40 oC) shows a high density of dislocation loops (left image), high density of H/He bubbles (center image) and presence of γ\'\' precipitates in SAD from z = [011] (right image).
Radiation induced-hardening is highest at the low dose region in the outer most edge. The hardening from γ\'\' precipitates is determined to be more pronounced than that from trapped bubbles. The lack of significant hardening in the highest dose region is attributed to a lower dis-location density and no γ” precipitates or bubbles [3]. Identification of H or He bubbles and the higher accumulation of these bubbles in the low dose region (no direct beam hitting) warrant further studies.
Despite the evidence of irradiation-induced hardening, this spent beam window appears to retain useful ductility after 5 years in service. At the conclusion of 2013 run cycle, the current in-service beam window had reached the same dpa as of the spent window. We plan to extend the service of the current in-service window until it reaches its intended design threshold limit of ~20 dpa (in the highest dose region). Additional measurements at higher dpa values will enable better decision-making in managing risks of the window failure
Einfluss von Biofilmen auf das Migrationsverhalten von Uran, Americium und europium in der Umwelt
Full text linkDie Mechanismen von Immobilisierungsprozessen radioaktiver Schwermetall-Ionen innerhalb von Biofilmen sind noch weitgehend unerforscht. Das liegt an der Komplexität der Biofilme, welche häufig diskrete geochemische Mikromilieus bilden, die sich vom umgebenden Milieu („Bulk Solution“) in Bezug auf dessen Biozönose (der mikrobiellen Diversität), den darin herrschenden geochemischen Bedingung (z.B. Red/Ox-Potential u./o. gelöster Sauerstoffmenge), aber auch in der Konzentration möglicher Komplexbildner (z.B. Metaboliten u./o. EPS-Komponenten) deutlich unterscheiden. Alle diese Faktoren können die Speziation der Radionuklide verändern und damit auch deren Transportverhalten. Für ein besseres Prozessverständnis zu den Wechselwirkungen von Radionukliden mit natürlichen, in Uran-kontaminierten Milieus lebende Mikroorganismen und den damit verbunden Stoffen wurde die Biozönose in Biofilmen und im Grubenwasser des ehem. WISMUT-Uranbergwerkes Königstein nach klassischen mikrobiologischen- und molekularbiologischen Methoden bestimmt. Aus einem Vergleich der Chemie im Biofilm mit der Chemie der umgebenden Lösung wird der Einfluss der Biofilme auf das Migrationsverhalten von Radionukliden in der Natur beurteilt. Die Identifizierung und Quantifizierung von Prokaryoten erfolgte u.a. mit der CARD FISH Methode. Die selektive Visualisierung der EPS-Komponenten in der Matrix der Biofilme wurde mit Hilfe der Konfokalen Laser Scanning Mikroskopie (CLSM) bewerkstelligt.
Zur Untersuchung der Speziation von fluoreszierenden Schwermetall-Ionen wie U(VI) kam die zeitaufgelöste, laser-induzierte Fluoreszenzspektroskopie (TRLFS) zum Einsatz. Um diese Methode auch im mikroskopischen Bereich anwenden zu können, wurde sie weiter zum CLSM hin entwickelt: Da ein 80-MHz-MaiTai-Laser zur Verfügung stand, wurde durch im kHz-Bereich alternierendes Beugen des Anregungslaserstrahls von der Probe weg (und wieder zu ihr hin) mittels akusto-optischem Modulator (AOM) eine quasi-gepulste Laseranregung im kHz-Bereich erreicht. Durch Einbindung von Frequenzvervielfachern („Harmonixx“ von APE Berlin und „Inspire“ von Spectra-Physics) konnte so eine gepulste Anregung innerhalb eines breiten Wellenlängenbereiches (ca. 230-1090 nm) ermöglicht werden. Für die Auswertung des als äußerst schwach zu erwartenden Fluoreszenzsignales (entsprechend des mikroskopisch kleinen Anregungsraumes) wurde die Time-Correlated Single-Photon Counting Methode (TCSPC) – auch „zeitbezügliche Einzelphotonenzählungs-Methode“ – an das Laser-Anregungssystem angepasst. Die Fluoreszenzlebenszeitkurve des Fluoreszenzsignals von U(VI) Species, die sich an der Oberfläche von den Protozoen Euglena Mutabilis befanden, konnte z.B. auf diese Art mit Hilfe der TCSPC ermittelt werden
Real-time beam-profile monitor for a medical cyclotron
Full text linkIntroduction
Measuring the beam profile on a medical cyclo-tron in real time can aid in improved tuning of the cyclotron and give important information for a smooth operation. Typically the beam profile is measured by an autoradiography technique or even by a scintillator that can be viewed in real time [1, 2]. Another method is to use collimators in front of the target to assess the beam center-ing [3]. All these methods have potential draw-backs including; an inability to monitor the beam in real time for the radiograph, exhibiting a non-linear correlation in signal response to the power deposited for a scintillator, and not providing a 2-dimensional profile of the complete beam for collimators. Our goal was to design a realtime, linear, 2-dimensional beam-profile monitor that is able to withstand the high power of a PET cyclotron.
Material and Methods
The beam-profile monitor (PM) is designed for the TR13, a 13MeV negative hydrogen-ion cyclotron at TRIUMF. The design follows the concept of a ‘harp’ monitor, widely used at TRIUMF for tuning proton and radioactive ion beams, and is installed on the extraction port without separation from the tank vacuum. The TR13 monitor is designed to withstand a 13 MeV proton beam with a beam current of up to 25 µA, has an active area of 10 by 10 mm and does not affect the 10-7 torr tank vacuum. The device consists of a water-cooled Faraday cup made out of aluminium for low activation and two orthogonal rows of eight tungsten electrodes each mounted on a water-cooled support frame. Electrodes are spaced 1 mm apart from each other, see FIG. 1. The electrodes are electrically isolated from each other and each has a current pickup soldered to it. The material and the shape of the electrodes are optimized to withstand the deposited power of the proton beam. A voltage of -90 V is applied to the electrodes to repel secondary electrons and prevent crosstalk between neighbouring electrodes. The electrode current is amplified using a custom current amplifier, and read by an ADC. From there, the current data is displayed on a PC. This allows one to observe changes of the beam profile in real time. The electronics are designed to read out all sixteen channels in parallel, or, if only a limited number of ADC channels are available, to cycle through the different channels. In our current setup all sixteen channels are read out simultaneously.
Results and Conclusion
The beam-profile monitor provides a real-time representation of the proton beam, see FIG. 2. The data can also be recorded and analyzed at a later time. The linearity of the monitor has been measured up to 30 µA of proton beam current [4]. With the use of the monitor, it was possible to increase the output of the ion source into the target by 50% in comparison to the standard tune
Isolation of 76Br from irradiated Cu276Se targets using dry distillation: evaluations and improvement for routine production
Full text linkIntroduction
76Br is of interest for in vivo PET imaging applications. Its relatively long half-life (16.1 h) allows use not only on small molecules but also proteins which have slow excretion as carrier molecules. Irradiation using a low energy proton beam (~ 20 MeV) on an enriched Cu276Se target, followed by dry distillation with thermal chromatography, is one of the best methods to obtain sufficient amounts of 76Br for clinical applications1,2. However, the thermal chromatography is plagued by poor reproducibility and appears unsuitable for automation of its production, leading us to remove the thermal chroma-tography from the dry distillation. In this investigation we employed H2O solution to collect 76Br and optimized the distillation condition using a small amount of 77Br (57.0 h). We also produced large amount of 76Br under the optimized conditions to evaluate the dry distillation method.
Material and Methods
Target preparation and dry distillation were conducted based on the methods described in previous reports1,2. To produce 77Br, Cu2natSe target was irradiated with 20 MeV proton beams (5 µA) accelerated by AVF cyclotron in the Japan Atomic Energy Agency. The following two systems were used in the dry distillation optimization studies; (1) an initial system was composed of two furnaces, a main and an auxiliary furnace. Temperature of each furnace was set at 1050 °C (main) and 200 °C (auxiliary) respectively; (2) the second system was made of one large furnace composed of heating and cooling area. Temperature of the heating area was varied from 1050 to 1120 °C. In both systems PTFE tubing, leading to a H2O solution (15 mL), was inserted into the apparatus. The irradiated target was heated under streaming Ar gas (30 mL/min.). An enriched Cu276Se target (76Se enrichment: 99.67%) was used for 76Br production. Radioactivity was measured on a high-purity germanium (HPGe) detector coupled to a multichannel analyzer. TLC analyses were conducted on Al2O3 plates (Merck) using 7:1 acetone:H2O as the eluting solvent.
Results and Conclusion
Low efficiency (33 %) of 77Br recovery was ob-served in the initial system. Distribution of radioactivity inside the apparatus showed that 35 % was trapped in the PTFE tube and the quartz tube. The recovery yield was increased up to 54 % when the auxiliary furnace was turned off, indicating that the temperature gradient inside the quartz tube is suitable to carry 77Br effectively to the H2O trap. We initially used a quartz boat to place the irradiated target in the furnace, but found that using a reusable tungsten backing was better. However, we found that recovery yield was dramatically reduced to 18 %. The studies where the temperature was varied showed that releasing efficiency was increased up to 100 % at the temperature of 1120 °C. Good recovery yield (~ 77 %) was achieved after optimizing the temperature gradient (FIG. 1b). Using the optimized setup, 76Br production runs (n = 6) have been conducted, allowing us to recover up to 39.8 MBq/µAh (EOB) of 76Br. High specific activity (~4400 GBq/µmol) was obtained in the final solution. TLC analysis showed that chemical form obtained was bromide. We concluded that the dry distillation using H2O trap is capable of providing enough high purity 76Br for clinical applications
Development and Characterization of a tunable ultrafast X-ray source via Inverse Compton Scattering
Full text linkUltrashort, nearly monochromatic hard X-ray pulses enrich the understanding of the dynamics and function of matter, e.g., the motion of atomic structures associated with ultrafast phase transitions, structural dynamics and (bio)chemical reactions. Inverse Compton backscattering of intense laser pulses from relativistic electrons not only allows for the generation of bright X-ray pulses which can be used in a pumpprobe experiment, but also for the investigation of the electron beam dynamics at the interaction point.
The focus of this PhD work lies on the detailed understanding of the kinematics during the interaction of the relativistic electron bunch and the laser pulse in order to quantify the influence of various experiment parameters on the emitted X-ray radiation.
The experiment was conducted at the ELBE center for high power radiation sources using the ELBE superconducting linear accelerator and the DRACO Ti:sapphire laser system. The combination of both these state-of-the-art apparatuses guaranteed the control and stability of the interacting beam parameters throughout the measurement.
The emitted X-ray spectra were detected with a pixelated detector of 1024 by 256 elements (each 26μm by 26μm) to achieve an unprecedented spatial and energy resolution for a full characterization of the emitted spectrum to reveal parameter influences and correlations of both interacting beams. In this work the influence of the electron beam energy, electron beam emittance, the laser bandwidth and the energy-anglecorrelation on the spectra of the backscattered X-rays is quantified.
A rigorous statistical analysis comparing experimental data to ab-initio 3D simulations enabled, e.g., the extraction of the angular distribution of electrons with 1.5% accuracy and, in total, provides predictive capability for the future high brightness hard X-ray source PHOENIX (Photon electron collider for Narrow bandwidth Intense X-rays) and potential all optical gamma-ray sources.
The results will serve as a milestone and starting point for the scaling of the Xray flux based on available interaction parameters of an ultrashort bright X-ray source at the ELBE center for high power radiation sources. The knowledge of the spatial and spectral distribution of photons from an inverse Compton scattering source is essential in designing future experiments as well as for tailoring the X-ray spectral properties to an experimental need.Ultrakurze, quasi-monochromatische harte Röntgenpulse erweitern das Verständnis für die dynamischen Prozesse und funktionalen Zusammenhänge in Materie, beispielsweise die Dynamik in atomaren Strukturen bei ultraschnellen Phasenübergängen, Gitterbewegungen und (bio)chemischen Reaktionen. Compton-Rückstreuung erlaubt die Erzeugung der für ein pump-probe-Experiment benötigten intensiven Röntgenpulse und ermöglicht gleichzeitig einen Einblick in die komplexen kinematischen Prozesse während der Wechselwirkung von Elektronen und Photonen.
Ziel dieser Arbeit ist, ein quantitatives Verständnis der verschiedenen experimentellen Einflüsse auf die emittierte Röntgenstrahlung bei der Streuung von Laserphotonen an relativistischen Elektronen zu entwickeln.
Die Experimente wurden am ELBE - Zentrum für Hochleistungs-Strahlenquellen des Helmholtz-Zentrums Dresden - Rossendorf durchgeführt. Der verwendete supraleitende Linearbschleuniger ELBE und der auf Titan-Saphir basierende Hochleistungslaser DRACO garantieren ein Höchstmaß an Kontrolle und Stabilität der experimentellen Bedingungen. Zur Messung der emittierten Röntgenstrahlung wurde ein Siliziumdetektor mit 1024x256 Pixeln (Pixelgröße 26μm × 26μm) verwendet, welcher für eine bisher nicht erreichte spektrale und räumliche Auflösung sorgt. Die so erfolgte vollständige Charakterisierung der Energie-Winkel-Beziehung erlaubt Rückschlüsse auf Parametereinflüsse und Korrelationen von Elektronen- und Laserstrahl.
Eine umfassende statistische Analyse, bei der ab-initio 3D Simulationen mit den experimentellen Daten verglichen und ausgewertet wurden, ermöglichte u.a. die Bestimmung der Elektronenstrahldivergenz mit einer Genauigkeit von 1.5% und erlaubt Vorhersagen zur zu erwartenden Strahlung der zukünftigen brillianten Röntgenquelle PHOENIX (Photon electron collider for Narrow bandwidth Intense X-rays) und potentiellen lasergetriebenen Gammastrahlungsquellen. Die Ergebnisse dienen als Fixpunkt für die Skalierung des erwarteten Photonenflusses der Röntgenquelle für die verfügbaren Ausgangsgrößen am Helmholtz-Zentrum Dresden - Rossendorf. Das Wissen um die räumliche und spektrale Verteilung der Röntgenstrahlung ist entscheidend für die Planung zukünftiger Experimente sowie zur Anpassung der Quelle an experimentelle Bedürfnisse
Thick target preparation and isolation of 186Re from high current production via the 186W(d,2n)186Re reaction
Full text linkRhenium-186 has a half-life (t1/2 = 3.72 days) and emission of both gamma and beta particles that make it very attractive for use as a theranostic agent in targeted radionuclide therapy. 186Re can be readily prepared by the 185Re(n,γ)186Re reac-tion1. However, that reaction results in low specific activity, severely limiting the use of reactor produced 186Re in radiopharmaceuticals. It has previously been shown that high specific activity 186Re can be produced by cyclotron irradiations of 186W with protons and deuterons2,3. In this investigation we evaluated the 186W(d,2n)186Re reaction using thick target irradiations at higher incident deuteron energies and beam currents than previously reported. We elected not to use copper or aluminum foils in the preparation of our 186W targets due to their activation in the deuteron beam, so part of the investigation was an evaluation of an alternate method for preparing thick targets that withstand μA beam currents. Irradiation of 186W. Initial thick targets (~600-1100 mg) were prepared using 96.86% enriched 186W by hydraulic pressing (6.9 MPa) of tungsten metal powder into an aluminum target support. Those thick targets were irradiated for 10 minu-tes at 10 µA with nominal extracted deuteron energies of 15, 17, 20, 22, and 24 MeV.
Isolation of 186Re. Irradiated targets were dissolved with H2O2 and basified with (NH4)2CO3 prior to separation using column(s) of ~100–300 mg Analig Tc-02 resin. Columns were washed with (NH4)2CO3 and the rhenium was eluted with ~80˚C H2O. Gamma-ray spectroscopy was per-formed to assess production yields, extraction yields, and radionuclidic byproducts.
Recycling target material. When tested on a natural abundance W target, recovery of the oxidized WO4- target material from the resin was found to proceed rapidly with the addition of 4M HCl in the form of hydrated WO3. The excess water in the WO3 was then removed by calcination at 800 °C for 4 hours. This material was found to undergo reduction to metallic W at elevated temperatures (~1550 °C) in a tube furnace under an inert atmosphere (Ar). Quanti-fication of % reduction and composition analyses were accomplished with SEM, EDS, and XRD and were used to characterize and compare both the WO3 and reduced Wmetal products to a sample of commercially available material. Structural enhancement by surface annealing. In some experiments ~1 g WO3 pellets were prepared from Wmetal that had been chemically treated to simulate the target material recovery process described above. Following calcination, the WO3 was allowed to cool to ambient temperature, pulverized with a mortar and pestle and then uniaxially pressed at 13.8 MPa into 13 mm pellets. Conversion of the WO3 back to Wmetal in pellet form was accomplished in a tube furnace under flowing Ar at 1550 °C for 8 hours. Material characterization and product composition analyses were conducted with SEM, EDS, and XRD spectroscopy. Graphite-encased W targets. Irradiations were conducted at 20 μA with a nominal extracted deuteron energy of 17 MeV using thick targets (~750 mg) of natural abundance tungsten metal powder uniaxially pressed into an aluminum target support between layers of graphite pow-der (100 mg on top, 50 mg on the bottom). Targets were then dissolved as previously described and preliminary radiochemical isola-tion yields obtained by counting in a dose calibrator. Although irradiations of W targets were possible at 10 μA currents, difficulties were encountered in maintaining the structural integrity of the full-thickness pressed target pellets under higher beam currents. This led to further investigation of the target design for irradiations conducted at higher beam currents. Comprehensive target material characterization via analysis by SEM, EDS, XRD, and Raman Spectroscopy allowed for a complete redesign of the target maximizing the structural integrity of the pressed target pellet without impacting production or isolation. At the 10 A current, target mass loss following irradiation of an enriched 186W target was < 1 % and typical separation yields in excess of 70 % were observed. Saturated yields and percent of both 183Re (t½ = 70 days) and 184gRe (t½ = 35 days) relative to 186gRe (decay corrected to EOB) are reported in TABLE 1 below. The reason for the anomalously low yield at 24 MeV is unknown, but might be explained by poor beam alignment and/or rhenium volatility during irradiation. Under these irradiation conditions, recovery yields of the W target material from the recycling process were found to be in excess of 90% with no discernable differences noted when compared to commercially available Wmetal and WO3. Conceptually, increasing the structural integrity of pressed WO3 targets by high temperature heat treatment under an inert atmosphere is intriguing. However, the treated pellets lacked both density and structural stability resulting in disintegration upon manipulation , despite the initially encouraging energy dispersive X-ray spectroscopy (EDS) determination that 94.9% percent of the WO3 material in each pellet had been reduced to metallic W.
The use of powdered graphite as a target stabi-lizing agent provided successful irradiation of natural abundance W under conditions where non-stabilized targets failed (20 µA at 17 MeV for 10 minutes). Target mass loss following irradiation of a natW target was < 1 % and a separation yield in excess of 97 % was obtained. In conclusion, the theranostic radionuclide 186Re was produced in thick targets via the 186W(d,2n) reaction. It was found that pressed W metal could be used for beam currents of 10 μA or less. For deuteron irradiations at higher beam currents, a method involving pressing W metal between two layers of graphite provides increased target stability. Both target configurations allow high recovery of radioactivity from the W target material, and a solid phase extraction method allows good recovery of 186Re. An effective approach to the recycling of enriched W has been developed using elevated temperature under an inert atmosphere. Further studies are underway with 186W targets sandwiched by graphite to assess 186Re production yields, levels of contaminant radiorhenium, power deposition, and enriched 186W material requirements under escalated irradiation conditions (20 µA and 17 MeV for up to 2 hours)
Proton irradiation of gold targets for 197(m)Hg production
Full text linkIntroduction
Irradiation of gold with protons provides access to no-carrier-added 197mHg and 197Hg. Interests in these radionuclides were awakened by the unique chemical and physical properties of mercury and its compounds combined with convenient nuclear properties like suitable half life (197mHg: T1/2 = 23.8 h, 197Hg: T1/2 = 64.14 h), low energy gamma radiations for imaging, Auger – and conversion electrons for therapy. The high thermal conductivity of gold enables high current irradiations and the monoisotopic natural abundance of 197Au supersedes expensive enrichment of the target material. The 197Au(p,n)197(m)Hg reaction was applied until now only for beam monitoring1, stacked foil meas-urements2 or very small scale tracer production.
Material and Methods
The irradiations were performed at a Cyclone 18/9 (IBA, Louvain la Neuve, Belgium). Its beam-line was sealed with a 1.0 mm vacuum foil (high purity aluminum, 99.999 %) from Goodfellow (Huntingdon, England). High purity gold disks (23 mm diameter, 2 mm thickness, 99.999% pure, 1 ppm Cu) as target material were purchased from ESPI (Ashland, USA). Gold foils as alternative gold targets (12.5×12.5 mm, 0.25 mm thickness, 99.99+ %, 1 ppm Cu) between an aluminum disk (22 mm diameter, 1 mm thickness, 99.0 %, hard) and an aluminum lid (23 mm diameter, 99.0 %, hard) were purchased from Goodfellow (Huntingdon, England). Hydrochloric acid (30%) and nitric acid (65%) were purchased from Roth (Karlsruhe, Germany) in Rotipuran® Ultra quality. Deionized water with > 18 MΩcm resistivity was prepared by a Milli-Q® system (Millipore, Molsheim, France). For separation of target material and side products a liquid-liquid extraction method (Gold was extracted with methyl isobutyl ketone (MIBK) from 2 M HCl target solution) and an ion exchange method (cation exchange resin (Dowex50W-x8, 100–200 mesh, H+ form) were applied.
Results and Conclusion
No-carrier-added 197(m)Hg was produced from gold via the 197Au(p,n)197(m)Hg reaction at proton energies of 10 MeV in sufficient quantity and quality for imaging studies.
Two different methods were studied for the separation of Hg radionuclides generated from Au targets. The results demonstrate the possibility to produce 197(m)Hg from gold at low proton energies. Combined with the presented radiochemical separation methods, the 197Au(p,n) reaction could be the basis for repeatable production of 197(m)Hg for imaging and therapy research on sufficient activity level
A Mini-PET beamline for optimized proton delivery to the ISOTRACE™ target system
Full text linkIntroduction
The ISOTRACE™ Super-Conducting Cyclotron is PMB-Alcen’s redeveloped and modernized version of Oxford Instrument’s OSCAR superconducting cyclotron [1]. Its extracted 80+ mi-croamperes of 12 MeV protons are used for the production of PET radioisotopes. Following the philosophy of Dickie, Stevenson, Szlavik [2] for minimizing dose to personnel, and as developed by Dehnel et al [3,4], and Stokely et al [5], the ISOTRACE™ shall utilize an innovative, light-weight, integrated and self-supporting Mini-Beamline. This permits the relatively high residual radiation fields around PET targets to be moved ~1 metre away from the cyclotron, and facilitates the use of local shielding (around the targets) that limits prompt gammas and neutrons, but more importantly attenuates the residual target radiation, so that maintenance/research staff can work on the cyclotron in a relatively low activity environment. In addition, the mini-beamline for PET utilizes a compound quadrupole/steerer doublet that permits active and dynamic focusing/steering of the extracted proton beam for optimized production and minimized losses [3], so it improves on the successful work of Theroux et al [6]. The integrated beamline unit is extremely small, so that it is very unlike bulky traditional PET and SPECT beamlines that require substantial support structures, such as described by Dehnel in [7,8].
Material and Methods
The ISOTRACE™ cyclotron is pictured in FIG. 1. The exit port flange and gate valve to which the integrated mini-beamline for PET shall be mounted is shown. Immediately upstream of the exit port, hidden from view, is a 4 jaw collimator (called BPI for Beam Position Indicator) with spilled beam current readbacks to the control system. TABLE 1 shows the nominal beam emittance and Twiss parameter values at the exit port flange location. This ion-optical information is necessary to simulate ion beam transport, develop the mini-beamline, and determine a nominal tune (i.e. magnet settings).
Results and Conclusion
TABLE 2 shows the ion-optical system parameters. FIGS. 2 and 3 show the horizontal and vertical beam profiles. The Horizontally focusing Quadrupole magnet (HQ), and Vertically focusing Quadrupole magnet (VQ) aperture diameter, 33 mm, was chosen to give sufficient beam acceptance. The focusing strength is a function of BL, so the effective length, L = 150 mm, was chosen to ensure Bmax less than 0.3 Tesla, while keeping overall magnet mass down. The quad-rupole magnets are fitted with water-cooled compound coils in which the copper/mylar strip wound portion of each coil is a winding for the quadrupole focusing function, and the wire wound portion is for the steering function. To increase beam acceptance and provide additional section strength for the pipe support function, the internal aperture of the low-activation aluminium beam pipe and the external shape are in the shape of a cross. FIG. 4 shows the beam crosssection at the mid-point of the downstream quadrupole magnet, and illustrates the additional acceptance as compared to a round beampipe. In order to machine the interior profile, the pipe is comprised of two premachined pieces that are friction stirwelded together. FIG. 5 is an isometric of the mini-beamline for PET.
The four upstream HQ compound coils are excited with a 75A power supply for the horizontally focusing quadrupole magnet function, and a ± 10A power supply for a vertical steering function. The same power supplies are used for the four downstream VQ compound coils for the purpose of a vertically focusing quadrupole magnet function and horizontal steering function
Operational measurements of 18F and 81Rb activities during transport
Full text linkIntroduction
Activity measurement of the produced radionuclide prior its transport to further processing in the clean rooms indicates proper irradiation settings and target functioning. It is particularly true for shortlived radionuclides. Precise online activity measurement of the radionuclides transported from the target to the hot cells in a liquid phase was highly desirable in order to estimate compliance with the required value. In this paper, we present simple operational systems for activity measurement of the irradiated enriched (18O) water for 18F labelled PET radiopharmaceuticals and 81Rb aqueous solution for manufacturing radionuclide generator 81Rb/81mKr.
Material and Methods
Irradiated aqueous solution (2.5 ml of enriched water with 18F up to 200 GBq) is transported via capillary to a synthesis module. Due to spreading out the liquid product on measuring vial walls, measured activity may vary up to 12 %. In order to avoid this variability, we have introduced simple system based on the measurement of several loops of the transporting capillary. The product is then evenly distributed around GM tube positioned in the loops’ centre. Typical GM tube response is displayed on FIG. 1.
The data are recorded and processed online. Maximum mean value of 20 consecutive values is calculated. The GM tube response was calibrated by precise activity measurement of the same product in a calibrated ionizing chamber (Atomlab). Calibration covers full range of the produced 18F activities.
Radionuclide 81Rb for the 81Rb/81mKr generator is produced via proton irradiation of pressurized enriched 82Kr gas. The product deposited on the target walls is washed out by water and transported to a container in a hot cell for filtration before transfer to a clean lab. The solution activity in the container (7–25 GBq) is measured with a GM tube in constant geometry. Typical response of the GM tube to the measured activity of 81Rb is displayed on FIG. 2. For activity determination, the mean value of 200 consecutive readouts starting from the 120th readout following maximum is used. The calibration for the whole range of the produced activities was performed via precise measurement of the cumulative 81Rb activity concentration by standard γ-spectrometry using HPGe detector.
Results and Conclusion
A simple operational system for online activity measurement of 18F and 81Rb in aqueous solutions using GM tube was designed, calibrated and implemented. Long term statistics show that the measured activities do not differ from the values obtained on calibrated ionizing chamber (18F) or γ-spectrometer (81Rb) for more than ± 2.5 %. The method seems to be cheap and rapid for reliable estimate of the produced activities online
Preparation of routine automated synthesis of [11C]choline
Full text linkIntroduction
[11C]choline is a very effective PET radiopharma-ceutical for the study of prostate cancer. To support the increasing demand for [11C]choline, several different synthetic approaches have been described in the literature, including different automated production methods using remote-controlled synthesis modules [1–4]. The most popular method uses a C18 Sep-Pak as solid support for methylation and, subsequently, a CM Sep-Pak for purification [2]. We report an optimized method for producing [11C]choline using only one CM Sep-Pak for both reaction and purification as was shown in the literature [4]. For synthesis of [11C]choline we used two modules Tracerlab FXC for preparation of methylation reagent [11C]CH3I and GPF-101 for [11C]choline synthesis.
Material and Methods
TracerlabFXC GE, GPF-101 Veenstra Instrument, 2-(dimethylamino)-ethanol (DMAE) ABX, Sep-Pak Light Accell Plus CM cation-exchange cartridges Waters used without conditioning, precursor 50 µL of DMAE dissolved in 25 µL of ethanol and loaded on a CM Sep-Pak. Schematic diagram of the automated system for the production of [11C]choline is given below. [11C]CH4 was produced in two standard Nitra target IBA irradiation of mixture 90 % N2/10 % H2 with 15 MeV protons using dual beam.
Results and Conclusion
[11C]CH4 was prepared in the targets and connected with Tracerlab FXC. [11C]CH3I was pre-pared in a loop in which allowed to react of elemental iodine at a temperature 720 oC. Con-version to [11C]CH3I usually is around 50% uncorrected activity. Activity is within the range 15–18 GBq of [11C]CH3I and time of production 10 min.
Synthesis of [11C]choline is based on the reaction DMAE with [11C]CH3I on a Accell Plus CM cation-exchange column which serves both as a support for reaction and for separation of choline from DMAE by ethanol washing. The basic parameters are shown in TABLE 1.
Beam current 2X 20 µA
Irradiation time 30 min
DMAE 50 µl
Synthesis time from EOB 25 min
Absolute yield without correction 6.6 GBq
Radiochemical purity > 99 %
Residual DMAE in product < 5 ppm
Ethanol < 1000 mg/L
pH 4.5–8.5
TABLE 1. Reaction parameters and result of production of [11C]choline syntheses
Conclusion
We have applied a simple synthesis method for [11C]choline preparation using automated commercial equipments with one column used both for reaction and separation purpose. The main advantage of using one column is lower contamination of the product [11C]choline with DMAE. When for synthesis of [11C]choline two columns C18 for synthesis and CM for separation is used, higher contamination of DMAE can be found in the product due to a release of DMAE from C18 column