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Saturation conditions in elongated single-cavity boiling water targets
Full text linkIntroduction
It is shown that a very simple model reproduces the pressure versus beam current characteristics of elongated single-cavity boiling water targets for 18F production surprisingly well. By fitting the model calculations to measured data, values for a single free parameter, namely an overall heat-transfer coefficient, have been extracted for several IBA Nirta H218O targets. IBA recently released details on their new Nirta targets that have a conical shape, which constitutes an improvement over the original Nirta targets that have a cylindrical shape [1,2]. These shapes are shown schematically in FIGURE 1. A study by Alvord et al. [3] pointed out that elevated pressures and temperatures in excess of the saturation conditions may exist in a water target during bombardment. However, as long as the rate of condensation matches the rate of vaporization, the bulk of the system should remain at saturation conditions. Superheated regions are therefore likely to form but also likely to disappear rapidly, typically on the scale of a few milliseconds. Even though the boiling process is generally quite complex, enhanced by radiation-induced nucleation, the presence of fast mixing mechanisms in the water volume justifies some simplifications to be made.
Materials and Methods
The simplified model assumes that the bulk of the target water has a constant temperature, which is the same as the inner wall temperature of the cavity, Tw. A second simplification is to neglect the temperature difference across the target chamber wall, which is only justified if the wall is thin. The boiling is not explicitly taken into consideration, including the rather complex boiling behaviour at the Havar window, except to acknowledge that it is the main mixing mechanism. Large temperature gradients can briefly exist in the water medium but they also rapidly disappear. A further assumption is that a single, overall convective heat-transfer coefficient can be applied, which is constant over the entire water-cooled surface. As the wall thickness is neglected, the heat-transfer surface is assumed to be the inner surface of the cavity, excluding the surface of the Havar window. One can then write down an energy balance between the beam heating and the convection cooling (Newton’s law of cooling), where Ib is the beam intensity, ΔE is the energy windows of the target (taken as 18 MeV), h is the convective heat-transfer coefficient, A is the inner cavity surface through which the heat has to be transferred from the target-water volume to the cooling water, and T0 is the cooling-water temperature. The saturated vapour pressure of water versus temperature is a characteristic curve, given by the steam tables [4]. Assuming the bulk of the system at saturation conditions, one gets from (1) and (2). The function f is represented by a polynomial. The only unknown in Equation (3) is the overall convective heat-transfer coefficient h. Our approach was to adjust h until a good fit with a set of measured data was obtained. It also has to be mentioned that subtle differences in the physical properties between 18O-water and natural water have been neglected. All in all, quite a few assumptions and simplifications are made in deriving Equation (3) and the system is, admittedly, much more complex. Nevertheless, the results obtained by applying Equation (3) are rather interesting.
Results and Conclusion
Measured data and corresponding calculations are shown in FIGURE 2 for three different conical targets and one cylindrical target. The extracted convective heat-transfer coefficients are pre-sented in TABLE 1 for the four cavities. As can be seen in FIGURE 2, while there are some differences between the data and calculated curves, especially towards lower beam currents, the overall agreement is remarkably good. It is possible that the better agreement towards higher beam intensities is related to more ebullient boiling and more rapid mixing, i.e. closer to the conditions that the model assumes. The values obtained for the overall convective heat-transfer coefficient are also remarkably similar. This tells us that, by and large, all the cavities perform in a similar way and the performance in terms of maximum operational beam current depends largely on the available surface to effectively remove the heat from. The values of h increase marginally if a smaller value is adopted for the cooling water. Note that the choice of T0 = 30 ᵒC used to obtain the results in TABLE 1 is typical for the room temperature closed-loop cooling system used at iThemba LABS, once it has stabilized under operational conditions.
A study by Buckley [5] on a quite different target design reports a value of h = 0.49 W cm−2 ᵒC−1, which is reassuringly similar. That study describes a cylindrical target cavity with a volume of 0.9 cm3, 8 mm deep, cooled with 25 ᵒC water from the back, operated with a 15 MeV proton beam with an intensity of 30 µA. The Nb Nirta targets are typically filled with 18O-water to about 60% of the cavity volume (see refs. [1,2] for the recommended values). The elongated shape, in combination with the ebullient properties of the boiling water, prevents burn-through. All the targets deliver the expected saturation yield. The targets are self-regulating ─ no external gas pressure is required. While the thermosyphon targets seemingly take advantage of a superior concept, we are now questioning whether this is really so in practice? It is not clear to us that the much more complex thermosyphon targets deliver any operational and/or performance advantages compared to the simple elegance of these elongated, single-cavity boiling target designs
Production of [11C]cyanide for the synthesis of indole-3-[1-11C]acetic acid and PET imaging of auxin transport in living plants: Production of [11C]cyanide for the synthesis of indole-3-[1-11C]acetic acid and PET imaging of auxin transport in living plants
Full text linkIntroduction
Since its development by Al Wolf and colleagues in the 1970s1, [11C]cyanide has been a useful synthon for a wide variety of reactions, most notably those producing [1-11C]-labeled amino acids2. However, despite its position as rote gas-phase product, the catalytic synthesis is difficult to optimize and often only perfunctorily dis-cussed in the radiochemical literature. Recently, [11C]CN– has been used in the synthesis of indole-3-[1-11C]acetic acid ([11C]IAA), the principal phytohormone responsible for a wide variety of growth and development functions in plants3. The University of Wisconsin has expertise in cyclotron production and radiochemistry of 11C and previous experience in the PET imaging of plants4,5. In this abstract, we present work on optimizing [11C]CN– production for the synthesis of [11C]IAA and the PET imaging of auxin transport in living plants.
Material and Methods
[11C]CH4 was produced by irradiating 270 psi of 90% N2, 10% H2 with 30 µA of 16.1 MeV protons from a GE PETtrace cyclotron. After irradiation, the [11C]CH4 was converted to [11C]CN– by passing through a quartz tube containing 3.0 g of Pt wire and powder between quartz wool frits inside a 800–1000 ˚C Carbolite tube furnace. The constituents and flow rate of the [11C]CH4 carrier gas were varied in an effort to optimize the oven\'s catalytic production of [11C]CN– from CH4 and NH3. The following conditions were investigated:
i. Directly flowing irradiated target gas versus trapping, purging and releasing [11C]CH4 from a −178 ˚C HayeSep D column in He through the Pt furnace.
ii. Varying the amount of anhydrous NH3 (99.995%) mixed with the [11C]CH4 carrier gas prior to the Pt furnace. Amounts varied from zero to 35 % of gas flow.
iii. Varying the purity of the added NH3 gas with the addition of a hydride gas purifier (Entegris model 35KF), reducing O2 and H2O impurities to < 12 ppb.
iv. Varying the flow rate of He gas carrying trapped, purged and released [11C]CH4.
After flowing through the Pt furnace, the gas stream was bubbled through 300 µL of DMSO containing IAA precursor gramine (1 mg), then passed through a 60×5 cm column containing ascarite to absorb [11C]CO2, followed by a −178˚C Porapak Q column to trap [11C]CH4 and [11C]CO.
After bubbling, the DMSO/gramine vial was heated to 140 ˚C to react the gramine with [11C]CN–, forming the intermediate indole-3-[1-11C]acetonitrile ([11C]IAN), which was subsequently purified by solid phase extraction (SPE). The reaction mixture was diluted into 20 mL water and loaded onto a Waters Sep-Pak light C18 cartridge, followed by rinsing with 5 mL of 0.1% HCl : acetonitrile (99 : 1) and 10 mL of the same mixture in ratio 95 : 5, and finally eluted with 0.5 mL of diethyl ether. The ether was subsequently evaporated under argon flow, followed by the hydrolysis of [11C]IAN to [11C]IAA with the addition of 300 µL 1 M NaOH and heating to 140 ˚C for 5 minutes. After hydrolysis, the solution was neutralized with 300 µL 1 M HCl and purified using preparative high-performance liquid chromatography (HPLC) using a Phenomenex Luna C18 (10μ, 250×10mm) column with a mobile phase acetonitrile : 0.1% formic acid in H2O (35 : 65) at flow rate of 3 mL/min. The [11C]IAA peak, eluting at 12 minutes, was collected and rotary evaporated to dryness, then again after the addition of 5 mL acetonitrile, followed by its reconstitution in 50 µL of water. Analytical HPLC was performed on the [11C]IAA before and after this evaporation procedure using a Phenomenex Kinetex C18 (2.6μ, 75× 4.6 mm) column with a linear gradient elution over 20 minutes of 10 : 90–30 : 70 (acetonitrile : 0.1% formic acid) at a 1 mL/min flow rate, eluting at 7.6 minutes.
The transport of [11C]IAA was monitored following administration through the severed petiole of rapid cycling Brassica oleracea (rcBo) using a Siemens microPET P4 scanner. Transport was compared following administration to the first true leaf versus the final fully formed leaf in plants with and without exposure to the polar auxin transport inhibitor naphthylphthalamic acid (NPA).
Results and Conclusion
Optimization of the [11C]CN– gas phase chemistry was performed using two key metrics for measuring conversion yield. First is the fraction of total produced radioactivity that trapped in the DMSO/gramine solution (denoted %DMSO), and second, the fraction of DMSO/gramine-trapped activity that was able to react with gramine to form [11C]IAN (denoted %CN–). Under certain conditions, the former of these metrics experienced significant losses due to unconverted [11C]CH4 or through combustion, forming [11C]CO2 or [11C]CO. The latter metric experienced losses due to production of incomplete oxidation products of the CH4-NH3 reaction, such as methylamine. Total [11C]CH4 to [11C]CN– con-version yields is reported by the product of the two metrics. It was initially hypothesized that the irradiation of a 90% N2, 10% H2 target gas would produce sufficient in-target-hot-atom-produced NH3 to convert [11C]CH4 to [11C]CN– in the Pt furnace. However, conversion yields were found to be low and highly variable, with 13 ± 8 % trapping in DMSO/gramine, 9 ± 9 % of which reacted as CN– (n = 15). While in disagreement with previous reports1, this is likely as a result the batch irradiation conditions resulting ammonia losses in the target chamber and along the tubing walls. Yields and reproducibility were improved when combining the target gas with a stream of anhydrous NH3 gas flow with conversion yields reported in TABLE 1. However, these yields remained undesirably low, potentially as a result of the 10% H2 carrier gas having an adverse effect on the oxidative conversion of [11C]CH4 to [11C]CN–. To remedy this, the irradiated target gas was trapped, purged, released in He and combined with NH3 gas before flowing through the Pt furnace. Initial experiments using 99.995% anhydrous NH3 gas resulted in very poor (< 0.1%) [11C]CN– yields as a result of nearly quantitative combustion forming [11C]CO2. Installation of a hydride gas purifier to reduce O2 and H2O impurities in NH3 improved yields for CH4 in He, but did not significantly affect those from [11C]CH4 in N2/H2 target gas. In disagreement with previous reports2, conversion yields were found to be highly sensitive to overall carrier gas flow rate, with lower flow rates giving the best yields, as shown in TABLE 1. Optimization experiments are continuing.
The total decay-corrected yield for the 1 hour synthesis of [11C]IAA in 50 µL of water is 2.3 ± 0.7 %, based on the total produced [11C]CH4 with a specific activity ranging from 1–100 GBq/µmol. The principal radiochemical impurity was determined to be indole-3-carboxylic acid. The SPE procedure isolating the [11C]IAN intermediate product was optimized to minimize this impurity in the final sample.
After a rapid distribution of the administered [11C]IAA through the cut petiole and throughout the rcBO plant, upward vascular transport of auxin and downward polar auxin transport was visualized through time-activity curves (TACs) of regions of interest along the shoot. Comparison of these TACS with and without exposure to NPA yields insight into the fundamental physiological process of polar auxin transport in plants.
In conclusion, the Pt-catalyzed oxidative conversion of [11C]CH4 and NH3 to [11C]CN– is a challenging process to optimize and highly sensitive to carrier gas composition and flow rate. Optimization for our experimental conditions yielded several results which disagreed with previous reports. [11C]IAA produced using [11C]CN– is well suited for PET imaging of polar auxin transport in living plants
Development of a forced-convection gas target for improved thermal performance
Full text linkIntroduction
The internal pressure experienced by a gas tar-get during irradiation is dependent on the beam energy deposited in the target, the beam cur-rent, and the thermal behaviour of the target. [1] The maximum beam energy deposited is a function of the cyclotron capabilities and the gas inventory within the target. The maximum beam current is limited by the pressure produced in the target and the ability of the target assembly to remain intact. This is also a function of the thermal behaviour of the target, which is difficult to predict a priori since it is dependent on such things as convection currents that occur during irradiation. We conducted bench tests with model gas targets with and without forced convection currents to observe the effect on thermal behaviour. Based on those results we constructed a prototype gas target, suitable for irradiation, with an internal fan assembly that is rotated via external magnets.
Material and Methods
Bench tests were conducted with cylindrical and conical target bodies of aluminum. A nickel-chromium heater wire was inserted into the gas volume through the normal beam entrance port (FIGURE 1) to heat the gas while water cooling was applied to the target body. The voltage and current of the heater coil was monitored along with the pressure inside the target and the water inlet and outlet temperature. In the case of tests with a driven fan blade either the voltage applied to the electric motor was monitored or the fan speed itself was recorded. By assuming the ideal gas law, the pressure gives the average bulk temperature and a global heat transfer coefficient can be calculated between the target gas and the cooling water. [2]
A cylindrical target body was constructed that incorporated a fan blade driven by an external motor. This assembly used a simple o-ring seal on the rotating shaft. This seal was not robust enough for any tests under beam conditions. A prototype design suitable for in-beam operation employs a propeller mounted on a rotating disc housing two samarium cobalt magnets and spinning on two micro-bearings which are constructed to operate in high temperature environments. The micro-bearings are mounted on a pin projecting from a plate welded to the back of the gas target to allow assembly of the fan mechanism prior to attachment to the body (FIGURE 2)
Increased target volume and hydrogen content in [11C]CH4 production
Full text linkIntroduction
High starting radioactivity is usually advantageous for producing radiopharmaceuticals with high specific radioactivity. However, the [11C]CH4 yields from N2-H2 gas target fall short from theoretical amounts, as calculated from the cross section for the well-known 14N(p,α)11C nuclear reaction1. The beneficial effect of increased target chamber temperature on [11C]CH4 yields has recently been brought forward by us2 and others3. In addition to the temperature effect, our attention has also been on the hydrogen content factor.
This study intends to examine the N2-H2 target performance in a substantially larger target chamber and at higher temperatures than our setup before and compare the results to the existing data.
Materials and Methods
Aluminium bodied custom design target chamber is used in fixed 17 MeV proton beam irradiations. Target chamber is equipped with heating elements and cooling circuit for temperature control. In addition to the target chamber body temperature, the target gas loading pressure and irradiation current can be varied.
The irradiation product is collected into an ad-sorbent trap that was immersed in a liquid argon cooling bath within a dose calibrator.
Results and Conclusion
Pursued data will show [11C]CH4 saturation yields (Ysat [GBq/µA]) at different irradiation and target parameters
GE PETtrace RF power failures related to poor power quality
Full text linkIntroduction
Anyone who has ever overseen the installation of a new cyclotron is aware of the importance of addressing the numerous vendor-supplied site specifications prior to its arrival. If the site is not adequately prepared, the facility may face project cost overruns, poor cyclotron performance and unintended maintenance costs. Once a facility has identified the space, providing sufficient power is the next step. Every cyclotron vendor will provide you with a set of power specifications, but meeting these specifications can be difficult, especially when the cyclotron is placed in an existing structure. The cyclotron is an interesting collection of power supplies providing power to sensitive electronic circuitry. It is not sufficient to just provide enough power; you must also provide quality power. It is hoped that our efforts to resolve our poor power quality problems will assist others as they replace aging cyclotrons in existing institutions whose power quality has degraded over the years.
The University of Iowa Hospitals and Clinics completed installation of a GE PETtrace 800 cyclotron in November 2011. Four months prior to installation, GE service personnel arrived to do a power assessment. The result was that we met their specifications, but with reservations. We could easily provide the quantity of power required, but the specification also states that GE recommends that primary power remain at 480 VAC ± 5%. GE service personnel attached a power quality analyzer to the cyclotron main power panel and determined that we did have some events of 7 to 8 % sag, but they were in-frequent, perhaps once or twice a week lasting 20 to 50 msec. Sags were confirmed to be the result of large non-linear loads elsewhere in the hospital. If these occurred during a run, they may shut down the cyclotron, specifically the RF power supply. Further investigation revealed the presence of harmonics on our power. Harmonics are the multiples of 60Hz power that are reflected back into your facility’s power grid from large motor drivers. Commercial air handler, water pump and fan motors often use variable frequency drives (VFDs) for proportional control to meet the changing facility demands. This pro-vides a significant on-going cost savings, but may play havoc with power quality throughout the institution.
Harmonic distortion is often quantified as a total harmonic distortion (THD) percentage. Though not specifically mentioned in the site-specifications, our experience here will show that it is important not to overlook harmonic distortion. Its effects can be varied, erratic and wide-spread throughout the cyclotron system. When asked, GE service referred us to IEEE standards for electrical systems and equipment which states that THD is recommended to be below 5 % for most applications, but below 3 % for sensitive settings including airports and hos-pitals1.
Mitigation of voltage sag and harmonic distortion is an expensive and complex topic. It is recommended that you consult with your cyclotron vendor to determine if there exists a field-tested solution. Additionally, you should consult a power systems specialist to do an audit of your building’s power system.
Material and Methods
Characterization of Power Quality: This was accomplished using a Hioki 3197 Power Quality Analyzer and a couple Dranetz PX-5 Power Xplorers. Each monitoring cycle logged data for about a week, which seemed to be about the limit for these units when logging both THD and surge/sag events down to the duration of a single 60Hz cycle. Analysis of the circuit diagrams and communication with GE engineers indicated that the main power contactors to the cyclotron RF system were dropping power to protect the system. The feedback for this shutoff is a detection signal from the front-end EHT (high-voltage generation) circuit that is set at a level to be representative of the 5% AC deviation specification.
RF Power System Contactors: Every time the contactors of the RF power distribution system are energized/de-energized, some arching occurs at the contact surfaces. This arching pits the contactor surfaces such that over time the contactor surfaces become irregular and potentially resistive. Since the RF protection circuit triggered by the EHT circuit is downstream from the contactors, it is not so hard to envision why the system becomes more sensitive over time2. Additionally, the harmonic distortion also exists on the AC voltage energizing the contactors. As a result, they may not actuate as smoothly (de-pendent of degree of harmonic distortion) and further hasten the normal rate of pitting of contactor surfaces.
Results and Conclusion
Within weeks of installation, we began to get RF power shutoffs. They were infrequent at first, but soon began to occur numerous times a week, then numerous times a day. At approximately 3 months post installation, it was often difficult to get through a standard 30 to 45 minute bombardment to make F-18 for our daily patient FDG doses. We limped along for over a year until the University was willing to invest in a solution to address our power problems.
Periodic Power Analyses: These analyses, per-formed over the next year, indicated that our power quality worsened in the winter and re-turned to functional levels in the summer. The instance of voltage sag remained approximately the same throughout the year (a few short sags per week), but the THD was down to 6 % in the summer and nearly 10% in the winter. This result, combined with RF shutdown tracking and lack of correlation between observed power sags and RF shutdowns, led us to the conclusion that our very high harmonic distortion combined with small power fluctuations (< 5 %) were the culprit.
Mitigation Planning: There are a number of power conditioning technologies, but imposing the need to remove both voltage sag as well as harmonic distortion, quickly narrows the field. What remains are the following options: 1) UPS line conditioner with batteries, 2) UPS line conditioner with flywheel or 3) motor-generator power isolator. Battery maintenance costs ruled out the UPS battery line conditioner. Of the remaining two, if you have the space, the motor-generator is the simplest and cheapest (favored by forward military hospital units). But for the space constrained user, like us, the UPS flywheel line conditioner became the preferred option.
Additionally, it was identified in a power audit that the THD was only 4% at the transformers connected directly to the local power utility company supply (upstream of load effect and harmonic distortion sources). This was to be expected as load effects and harmonic distortion are worse if your tie-in point to the building power grid is at the same level or downstream of their sources. Additionally, a test was performed during a hospital backup generator test, wherein the suspected primary offenders (large motors and VFDs) were diverted to backup. As a result, the THD measured at the cyclotron primary power panel dropped by 2.5 %.
Working with University electricians, an outside power consultant, GE engineering and University Hospital Radiology Engineering, a two phase plan was created.
Phase 1: With a repurposed utility transformer, the cyclotron and PET cameras got their own dedicated transformer connected to the main utility power feed. We also replaced the old contactors in the RF power distribution system. Since installation, the measured THD has remained at 4.5 to 5 % year round and the sag incidence and magnitude are slightly improved.
Phase 2: With a quote from GE for a flywheel UPS we should be able to fully condition the power entering our facility, removing the load effect voltage sags as well as the harmonic distortion.
One year of operation after Phase 1 implementation, it has been decided that Phase 1 was all that was required. We haven’t had a single new instance of RF shutdown since
Quality assurance of 61Cu using ICP mass spectroscopy and metal complexation
Full text linkIntroduction
61Cu (T1/2 = 3.33 hr, Eβ= 1.22 MeV, 61.4 %) is an attractive isotope for positron emission tomography (PET) radiopharmaceutical agents such as ATSM and PTSM. Various separation processes have been reported for the production of 61Cu on a medium cyclotron using 13–22 MeV protons on natural and enriched 64Zn target materials [1,2].
This work, investigates production of 61Cu using both natural and enriched 64Zn targets and its separation. Three types of resins were used to assess for their efficiency and speed to separate the desired 61Cu from the 66,67,68Ga and 64Zn and for the recycling of 64Zn target material. The effective specific activity of purified 61Cu, was determined by ICP-MS and its titration with various polyaza and polycarboxylate complexing ligands.
Material and Methods
1. Production and Separation
Targets were irradiated by proton beam of IBA cyclotron 18/18MeV via the 64Zn(p,α) 61Cu and natZn(p,x) 61Cu reactions using an enriched 64Zn foil(15×15×0.05mm, ~50 mg) and natural foil (diameter 25 mm, 0.05 mm,~ 60 mg). Thirty minute irradiations were conducted with incident proton energies between 11.7–12.0 MeV and beam currents of 20 and 40 µA. Irradiated Zn targets were dissolved in 8M HCl at 150 oC then evaporated to dryness. Trace water to the resultant residue (twice) and resultant solutions evaporated to dryness. The residue was re-dissolved in 2ml of 0.01M HCl before loading onto a Cu-resin column (FIG. 1) Zn and Ga isotopes were collectively eluted using 30 ml of 0.01M HCl. The Cu was then removed using 1.5 ml of 8M HCl and passed directly onto a cation exchange followed by an anion exchange column. An additional 3 ml of 8M HCl was used to rinse the cation exchange column and ensure quantitatively removal of Cu (II) ions. The Cu was finally eluted from the anion exchange column using 3 ml of 2M HCl. The Cu solution was heated up at 150 oC until evaporated to dryness and 61Cu final product dissolved in 400–800 μL of 0.01M HCl.
2. Specific activity of 61Cu
The specific activity (GBq/µmol) of the purified 61Cu was determined by ICP-MS and compared with that determined using dota, nota and di-amsar complexing ligands.
For each 61Cu production run aliquot of final solution (100 µL) was left to decay before dilut-ing to 10 mL with 10% HNO3. Decayed samples were sent to ChemCentre (Curtin University) for ICP-MS analysis. Each sample was analysed for Cu, Al, Ca, Co, Fe, Ga, Ni, Si, and Zn, which are known to compete with Cu2+ for ligand complexation.
Effective specific activity of the 61Cu was deter-mined by titrating various known concentration of ligands with 61Cu solution. The method is detailed in the literature [3]. Briefly, varying concentrations of each ligand was prepared in 0.1M sodium acetate buffer pH 6.5 to a total volume 20 µL. Fixed concentration of diluted 61Cu (0.01M HCl) in 10 µL was added to each ligand solution. The mixtures were vortexed then left to incubate at the room temperature for 30 mins. Two uL aliquots were withdrawn (in triplicate) from each reaction mixture and spot-ted on ITLC –SA. [Mobile phase: 0.1M NaCl: 0.1M EDTA (9:1) for Cu2+ and diamsar mixtures: Rf 0.8 free Cu2+ and 0.1M sodium acetate pH 4.5: H2O: MeOH: ammonium hydroxide (20:18:2:1 v/v) for Cu2+ dota and nota mixtures: Rf >0.8 Cu-dota and Cu-nota Rf < 0.2 free Cu2+]. Complexation of the 61Cu with each ligand was complete within 30 mins at room temperature. Concentration of Cu2+ was deter-mined from the 50% labelling efficiency.
Results and Conclusion
1. Production and Separation
The radioisotopes production from natZn target must be minimized by the optimum proton energy to reduce a radiation dose in the final product. The excitation functions of 66,67,68Ga ,65Zn and 61Cu are shown in FIG. 2. Proton beam energy of 11.7 MeV was used for both Zn targets to minimise the production of Ga isotopes and prevent formation of 65Zn. For the enriched 64Zn target (99.30%) higher proton energy could be used for the production of 61Cu allowing for increased yields and reduce radio contaminants. Previously, we used anion and cation exchange resin as described in the literature to separate the 61Cu [1]. Unfortunately the literature method was too long (up to 3 hours) and requiring high concentration of HCl and long evaporation times compromising achievable yields [4]. Thieme S. et al., 2013 [2] reported the successful use of Cu-resin for the separation of Cu radioisotopes and it was of interest to the current work to test this material for the separation of 61Cu in our hands.
A cation, anion exchange and Cu-resin were combined into closed system to separate the 61Cu within 30 mins (FIG. 1). The system is designed to contain the transfer of solutions be-tween each column using simple plunger to force solution through and between each column. This system afforded an easy, reliable and fast separation of 61Cu that could be completed within 30 min.
2. Specific activity
The specific activity of 61Cu was determined using ICP-MS and by titration with three ligands is summarized in TABLE 1. The ICP-MS data show values ranging from 9.2 to 32.4 GBq/μmol for 8 production runs. Specific activity determine using nota and dota were in all cases lower than the ICP MS data indicating some interference from the other metal ion contaminates such as Fe(ii/Iii), Ni (II), Ca (II), Zn (II), Ga (III). The specific activity determine using diamsar, which is known to be highly selective for Cu(II) (and Zn(II) and Fe(III)) in the presence of alkali and alkaline earth ions gave values significantly higher effective specific activity than that obtained using ICP MS. Variations in values can be explained by presence of contaminating metal ions
Data compilation and evaluation for U(IV) and U(VI) for the Thermodynamic Reference Database THEREDA
Full text linkTHEREDA (Thermodynamic Reference Database) is a collaborative project, which has been addressed this challenge. The partners are Helmholtz-Zentrum Dresden-Rossendorf, Karlsruhe Institute of Technology (KIT-INE), Gesellschaft für Anlagen- und Reaktorsicherheit Braunschweig mbH (GRS), TU Bergakademie Freiberg (TUBAF) and AF-Consult Switzerland AG (Baden, Switzerland). The aim of the project is the establishment of a consistent and quality assured database for all safety relevant elements, temperature and pressure ranges, with its focus on saline systems. This implied the use of the Pitzer approach to compute activity coefficients suitable for such conditions. Data access is possible via commonly available internet browsers under the address http://www.thereda.de.
One part of the project - the data collection and evaluation for uranium – was a task of the Helmholtz-Zentrum Dresden-Rossendorf. The aquatic chemistry and thermodynamics of U(VI) and U(IV) is of great importance for geochemical modelling in repository-relevant systems. The OECD/NEA Thermochemical Database (NEA TDB) compilation is the major source for thermodynamic data of the aqueous and solid uranium species, even though this data selection does not utilize the Pitzer model for the ionic strength effect correction. As a result of the very stringent quality demands, the NEA TDB is rather restrictive and therefore incomplete for extensive modelling calculations of real systems. Therefore, the THEREDA compilation includes additional thermodynamic data of solid secondary phases formed in the waste material, the backfill and the host rock, though falling into quality assessment (QA) categories of lower accuracy. The data review process prefers log K values from solubility experiments (if available) to those calculated from thermochemical data
Annual Report 2014 - Institute of Resource Ecology
Full text linkThe Institute of Resource Ecology (IRE) is one of the eight institutes of the Helmholtz-Zentrum Dresden – Rossendorf (HZDR).
The research activities are mainly integrated into the program “Nuclear Waste Management, Safety and Radiation Research (NUSAFE)” of the Helmholtz Association (HGF) and focused on the topics “Safety of Nuclear Waste Disposal” and “Safety Research for Nuclear Reactors”.
Additionally, various activities have been started investigating chemical and environmental aspects of processing and recycling of strategic metals, namely rare earth elements. These activities are located in the HGF program “Energy Efficiency, Materials and Resources (EMR)”. Both programs, and therefore all work which is done at IRE, belong to the research sector “Energy” of the HGF.
The research objectives are the protection of humans and the environment from hazards caused by pollutants resulting from technical processes that produce energy and raw materials. Treating technology and ecology as a unity is the major scientific challenge in assuring the safety of technical processes and gaining their public acceptance. We investigate the ecological risks exerted by radioactive and nonradioactive metals in the context of nuclear waste disposal, the production of energy in nuclear power plants, and in processes along the value chain of metalliferous raw materials. A common goal is to generate better understanding about the dominating processes essential for metal mobilization and immobilization on the molecular level by using advanced spectroscopic methods. This in turn enables us to assess the macroscopic phenomena, including models, codes, and data for predictive calculations, which determine the transport and distribution of contaminants in the environment
Development of Cyclotron Radionuclides for Medical Applications: From fundamental nuclear data to sophisticated production technology
Full text linkSoon after the discovery of radioactivity it was shown that radionuclides can be used both for diagnostic and therapeutic studies, depending on the characteristic radiations emitted by them. By 1960’s the radionuclide production technology using nuclear reactors was well established. In early 1970’s a renaissance of the cyclotrons occurred because many of the neutron deficient radionuclides could only be produced using irradiations with charged particles, like protons, deuterons, α-particles, etc. Initially, interest was directed towards radioactive gases for inhalation studies and other radionuclides for scintigraphy. Later, with the advent of emission tomography, i.e. Single Photon Emission Computed Tomography (SPECT) and Positron Emission Tomography (PET), the emphasis shifted to 123I and positron emitters [cf. 1–3], and tremendous progress ensued. In order to keep abreast of the fast developments, a Symposium was organized at the Brookhaven National Laboratory (BNL), USA, in 1976, with the title “Radiopharmaceutical Chemistry”. This became a biennial event, with alternate meetings in North America and Europe. It included all aspects of radionuclide and radiopharmaceutical research. About a decade later, however, it was realized that for discussion of technical aspects, a separate forum would be more appropriate. A group of experts therefore convened the first Targetry Workshop in Heidelberg in 1985. Thereafter it was established as a recurring Workshop, with its scope enlargened to include also nuclear and radiochemical problems. Today, the major conference on Radiopharmaceutical Sciences and the specialist International Workshop on Target-ry and Target Chemistry are held in alternate years. The present Workshop is No. 15 in the series and it is being jointly held by the research groups in Dresden and Prague, both of which have a long tradition of cyclotron production of radionuclides. In this talk, some personal reminiscences and impressions of the historical de-velopments in the field over the last 40 years will be briefly described