Pushing the Limits of an O-18 Water Target J.A. Nye, D. W. Dick, and R.J. Nickles Department of Medical Physics, University of Wisconsin, Madison, Wisconsin. Abstract. A gridded-niobium target was constructed for the improvement of routine [18F]-fluorine production from 18Oenriched water on a CTI RDS 112 cyclotron. Niobium was chosen for its inertness and excellent thermal properties. The target volume consists of a 400µL (active volume) niobium chamber mounted with a single entrance foil supported against an array of 3mm hexagonal holes with 0.25mm aluminum septa, machined by EDM. The target operates at high beam currents and elevated pressures and temperatures with significant reductions in maintenance intervals. Several diagnostic tools such as autoradiography, activation, and neutron logging optimize the performance and yield of the target. Entrance foils including Havar and Nb are used to assess the [18F] chemical compatibility, with FDG synthesis as the test reaction. The gridded, single-foiled niobium target chamber appears to be an improvement compared to a standard double-foiled helium cooled water target used with RDS cyclotrons. Construction of a target using niobium relies on a sufficient heat dissipation rate on the foil side to overcome the inadequate thermal conductivity of the water filled target chamber. To improve the burst pressure of a niobium foil, the entrance foil can be mounted on a grid made of a high thermally conductive material such as aluminum or copper (3). Subsequently, the grid will provide mechanical strength allowing the pressure in the target volume to be increased. An increase in pressure will raise the boiling temperature and minimize the loss of useful beam from the formation of voids in the target chamber. INTRODUCTION Small volume water targets for the production of aqueous [18F]-fluoride have yet to be firmly established in a small clinical and research setting. Several performance limitations prevent small volume targets from operating reliably at beam currents of greater than 30µA. Insufficient heat dissipation from the target foil and target body limits beam currents, thereby increasing the required irradiation period. In addition, boiling and water voids formed within the target volume reduce yields and place unwanted stress on the inner surfaces of the target chamber. The most significant rate-limiting step in a small volume design is preventing the loss in reactivity of the [18F]-ion caused by contaminates from both the target body and knock-on ions created by surfaces in the beam strike. Therefore, the challenge presented is how to increase beam currents while minimizing losses in target performance due to inadequate heat dissipation and formation of reactive ions. METHODS AND DISCUSSION A small volume target is constructed by machining a 400µL active chamber in a niobium cavity mounted on a copper plate. Access to the target volume is accomplished with two silver-induction brazed 0.5mm I.D. stainless steel tubes. A circulating water cavity machined in the copper plate actively cools the area directly behind the niobium chamber. The copper plate used to mount the niobium chamber is 20mm deep with 3mm bored channels cut in the radial direction allowing access to the stainless tubing leads from the target’s exterior. A single entrance foil is mounted on Niobium is the material of choice in reactive environments because of its high melting point and chemical resistiveness (1). Other favorable materials are titanium and silver (2), however, silver targets are known to require frequent cleaning due to ion contamination. Titanium is a suitable counterpart to niobium but it is more difficult machine and has lower yield strength and heat conductivity. CP680, Application of Accelerators in Research and Industry: 17th Int'l. Conference, edited by J. L. Duggan and I. L. Morgan © 2003 American Institute of Physics 0-7354-0149-7/03/$20.00 1098 an aluminum grid consisting of a hex-hole array (3mm across the flats, 0.25mm septa, 12mm in axial depth). The grid is actively cooled by parallel-opposed water lines. FIGURE 2. Audioradiograph images of 65Zn produced from the reaction 65Cu(p,n)65Zn by bombarding natural 1mm thick copper foil in place of the Havar window. The top images show activation of the copper foil without the grid (top left) and with the grid (top right). The graphs below each image show the beam profile along a bisecting line without the grid (bottom left) and with the grid (bottom right). The beam profiles are normalized to their peak values for presentation purposes. FIGURE 1. Sectional view of the target assembly showing the placement of the grid and niobium target cell. The niobium chamber (bottom left) has a small head spaced machined on the outside perimeter of the beam strike area to act as a recombination space. The grid is shown in grayscale and a frontal view is shown under the sectional assembly (bottom right). It is evident from the above figure that a significant portion of the beam current enters through the center holes. This would suggest that further optimization of the grid would require an asymmetric hex-hole pattern to improve beam transmittance reducing the amount of beam lost on the septa. Furthermore, a diverging hexhole pattern, characteristic of the beam emittance, would also increase the transmittance. However, these modifications would only provide a small increase in overall performance. The aluminum grid is designed (4) for a bursting pressure of 2000psi for a 0.025mm havar foil. The open projected area is 85%. The incident beam profile of the CTI RDS 112 is defined by 1cm diameter entrance slits, with 6-8mm FWHM, resulting in a beam transmittance of 80% with the grid in place. Figure 2 shows a section profile of the incident beam on the target produced by activation of copper foil. Neutron logging during irradiation at pressure intervals from 400psi to 1500psi using H2natO and 10% enriched H218O water remain constant at beam currents ranging from 10-45µA. A constant neutron production rate suggests, even in the presence of boiling, the target water is still ‘thick’. Gamma spectroscopy using a heavily collimated BGO crystal post irradiation showed no evidence of 93mMo (γ=685keV, t1/2=6.95hr), from the reaction 93Nb(p,n)93mMo, produced in the target cell. Since the target’s inauguration in June 2002, the grid and Havar combination has operated without failure at currents of 45µA and pressure ranges from 400-1400psi. In order to increase the reactivity of eluted [18F]-fluoride an ion exchange column is used to decouple contaminant ions deposited in the target 1099 TABLE 1. Yield measurements for 94.6% enriched H218O water using a 0.025mm Havar foil. Interchanging the Havar with Nb foil results in similar yields. The target is operated with a total volume of 800µL, which includes the beam strike volume and associated fittings. The target over pressure in column three is helium gas. water during irradiation. FDG labeling yields are consistent at 60-65% decay-corrected using the Hamacher procedure (5). To improve the FDG labeling phase, a 0.025mm Nb-foil has recently replaced the Havar foil creating a complete Nb-target. The target is limited to pressures less than 450 psi as a result of niobium’s mechanical properties. The target has operated with the niobium foil at beam currents >30µA without foil failure and FDG labeling yields have increased to 70-75% decay corrected. Subsequent gamma spectroscopy on a natural water sample irradiated for >2 hours shows little to no measurable evidence of the primary contaminant, 93mMo. Figure 3 is data taken on a heavily shielded 10atm Xe well-detector capable of measuring activity at levels of >10nCi. Beam Current [µA] Bmb. Duration [min] Pressure [psi] Activity at EOB [mCi] Saturation Yield [mCi/µA] 13 117 400 715 101.3 13 125 400 730 102.9 20 107 500 1003 102.0 20 74 1100 725 100.2 CONCLUSION Development of a reliable low-maintenance water target for routine production of aqueous [18F]-fluoride is presented. The use of a niobium target insert and entrance foil has increased FDG labeling yields compared to a double-foiled (He cooled) silver target. The current limit for the Havar foil combination has yet to be reached. The target design allows the user to exchange target chambers (niobium, silver, titanium) and foil arrangements. Adaptation to flow through targetry for the production of [13N]-ammonia further demonstrates the versatility of the target. Total production expenses for the gridded target are approximately $2500. FIGURE 3. A six decade decay of H2natO after approximately two hours of irradiation with the Nbfoil. Saturation yields for the niobium target are limited by the grid transmittance. The thick target yield is approximately 100mCi/µA, table 1, and agrees with an 80% transmittance for thick H218O yields (6). Presently, the target has operated without a foil change or cleaning for 93hrs at an average beam current of 20µA. Normal operating conditions are 20µA for durations of approximately 120min with the Nb foil. One accidental irradiation occurred with no water cooling on the aluminum grid at a current of 20µA for 150min. Some heat damage occurred on the beam side of the grid but no serious harm is evident. ACKNOWLEDGEMENTS The authors of this paper would like to acknowledge Andrew Roberts and Todd Barnhart for their assistance in FDG synthesis. REFERENCES 1. Zeisler S. K., Becker R. A., Pavan R. A., Moschel R., and Rühle H., Appl. Radiat. Isot. 53, 449-453 (2000). 1100 2. Mulholland G. K., Hichwa R. D., Kilbourn M.R., and Moskwa J., J.Labelled Compd. Radiopharm. 26, 192-193 (1989). 3. Nickles R.J., Nucl. Instr. Meth. 177, 593-594 (1980). 4. Young W. G., Roark’s Formulas for Stress and Strain 6th ed., New York: McGraw-Hill, 1989, pp. 477-478. 5. Hamacher K., Coenen H. H., and Stocklin G., J. Nucl. Med. 27, 235-238 (1986). 6. Ruth, T.J. and Wolf A.F., Radiochem. Acta 26, 21-24 (1979). 1101
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