Thesis (Ph. D.)--University of Missouri-Columbia, 1998. / Typescript. Vita. Includes bibliographical references (leaves 134-139). Also available on the Internet.

Thesis (Ph. D.)--University of Texas at Austin, 2000. / Vita. Includes bibliographical references. Available also in a digital version from Dissertation Abstracts.

Thesis (Ph. D.)--Florida State University, 2004. / Advisor: Dr. Alan G. Marshall, Florida State University, College of Arts and Sciences, Department of Chemistry and Biochemistry. Title and description from dissertation home page (viewed June 16, 2004). Includes bibliographical references.

Thesis (Ph. D.)--University of Missouri-Columbia, 1998. / Typescript. Vita. Includes bibliographical references (leaves 134-139). Also available on the Internet.

Introduction Monte-Carlo simulations can be used to assess isotope production on small medical cyclotrons. These simulations calculate the particle interactions with electric and magnetic fields, as well as the nuclear reactions. The results can be used to predict both yields and isotopic contaminations and can aid in the optimum design of target material and target geometry [1,2]. FLUKA is a general-purpose tool widely used in many applications from accelerator shielding to target design, calorimetry, activation, dosimetry, detector design, neutrino physics, or radiotherapy [3,4]. In this work, we applied the Monte-Carlo code FLUKA to determine the accuracy of predicting yields of various isotopes as compared to experimental yields. Material and Methods The proton beam collimation system, as well as the liquid and solid target of the TR13 cyclotron at TRIUMF, has been modeled in FLUKA. The proton beam parameters were initially taken from the cyclotron design specifications and were optimized against experimental measurements from the TR13. Data from irradiations of different targets and with different beam currents were collected in order to account for average behavior, see FIG. 1. Yields for a pencil proton beam as well as a beam spread out in direction and energy have been calculated and have been compared to experimental results obtained with the TR13. Results and Conclusion The reactions listed in TABLE 1 were assessed. For most reactions a good agreement was found in the comparison between experimental and simulated saturation yield. TABLE 1 only shows the yields simulated with a proton beam with a spread in both direction and energy. In most cases, the simulated yield is slightly larger or comparable. Only the calculated yield for 55Co was significantly lower by a factor of 4.2. This is still a good agreement considering that FLUKA was originally a high-energy physics code. It may indicate that the FLUKA internal cross-section calculation for this isotope production needs some optimization. In summary, we conclude that FLUKA can be used as a tool for the prediction of isotope production as well as for target design.

Introduction The established methods for the production of 99Mo, based on fission in nuclear reactors, continue to present problems as a result of the plant’s aging and the significant investments needed for maintenance or for their renewal. Much research work is thus in progress on the study of alternative methods for the production of 99mTc in quantities and with the degree of purity required for the clinical use. Between them, the cyclotron production of 99mTc via the 100Mo(p,2n)99mTc reaction has turned out as the most attractive alternative. One critical aspect regarding the production of 99mTc with cyclotron is the need for a robust and reliable target production process. Several techniques have been indicated as extremely promising such has plasma spray and laser cladding; however these methods require specialized instrumentation and complex operations to be performed handling activated materials in order to recover irradiated Mo. In this work we report the development of the work done at the University of Bologna, as a part of a wider INFN project, as regards the methods of preparation of solid targets suitable for the production of 99mTc irradiating a target of 100Mo, employing a cyclotron for biomedical use, normally operated for the production of PET radionuclides. Material and Methods Irradiations were performed with a 16.5 MeV GE PETtrace cyclotron equipped with a solid target station previously developed by our group (1). In initial tests, a stack of 1–3 metallic foils, 100 μm thick, of natMo were irradiated with protons in the 15.9→9.8 MeV energy range. Foils were then dissolved in a HNO3-HCl solution and samples were analyzed with high resolution gamma-ray spectrometry (Canberra, including a HPGe detector with a 30% relative efficiency and a resolution of 1.8 keV at 1332 keV) using Genie2000 software; the measurement campaign lasted several weeks to take into account the different half-lives of the produced radionuclides. Results were extrapolated to a highly enriched 100Mo target and compared to Monte Carlo simulations previously performed with FLUKA and TALYS codes (2). In order to investigate a method of preparation of the target that would make easier the recovery of the enriched material and recycling for the preparation of a new target, it was subsequently studied the preparation of pellets of Molybdenum trioxide. MoO3 powder (Sigma Aldrich, 99.9% trace metals basis, particle size < 150 μm) was used to prepare pellets using a 10 ton press. Pellets obtained in this way were then sintered on a Platinum support using a CARBOLITE furnace under a controlled atmosphere; the temperature was ramped according to a controlled and reproducible temperature cycle. Sintered pellets were subjected to visual inspection, mechanical tests of resistance to loading and downloading in the cyclotron target station, thermal tests and then irradiated at increasing current. The irradiated targets were again visually inspected then weighed, dissolved and subjected to gamma-ray spectrometry analysis. Results and Conclusion The experimental saturation yield for 99mTc calculated on the basis of the gamma-ray analysis of irradiated metal foils, gave an extrapolated yield of 1.115 ± 0.015 GBq/μA for a 100 μm thick 100Mo enriched target, in accordance with the value of 1.107 ± 0.002 GBq/μA obtained in Monte Carlo simulations. On these bases, an irradiation of 3 h at 50 μA is expected to produce 16.3 ± 0.2 GBq of 99mTc; considering the use of an efficient purification system, a radionuclidic purity > 99.9 % 2 h after the EndOfBombardment and a specific activity comparable with the actual standards are expected as achievable. Experiments on sintering pellets are still on going at the time of writing this report; initial results showed that addition of proper aggregating materials allows for suitable pellets preparation. The sintering process allows to obtain pellets having sufficient mechanical strength to withstand loading and downloading operations. Initial irradiation tests with beam current up to 25 μA were performed successfully with no changes in mass and mechanical properties of the pellet. These encouraging results suggest that sintered pellets may be a relatively inexpensive and easy solution to prepare 100Mo targets for the cyclotron production of 99mTc. Further experimental tests at higher beam current will be performed in order to assess the maximum current achievable with no damage of the target. At the same time, a prototype automated module based on standard industrial components is in testing phase as regards performance in the separation and purification processes.

Introduction The worldwide use of PET has proven beyond dispute the importance for both routine diagnosis and physiological, oncological and pharmacological research. In many ways the present success of PET relies on the mature technology of PET compact medical cyclotrons. As long time developers of new targets, isotopes and com-pounds, we have been inclined to look for new block-buster applications, high power targets and sustainable ways of embracing the GMP and regional distribution, but recent pioneering development [1] around very small cyclotrons and “embedded synthesis and qc” has pointed out an old, but important nuclear physics lesson now halfway forgotten: that many PET isotopes can be made in high yields with proton energies far below 10 MeV [2]. This has opened a new interest in small cyclotrons and their targets. We have been testing the first GE Healthcare Prototype for a 7.8 MeV negative ion, internal ion source cyclotron with 3 production targets mounted on a short beamline. Here we present the first experimental yields of some of the important PET radionuclides. Materials and methods The prototype cyclotron (FIG. 1) has been in-stalled and tested without self-shield in designated experimental area in order to establish the neutron field around accelerator and targets in order to qualify design calculations for a future integrated shield. The cyclotron energy is fixed by the radial position of the extraction foil, while the azimuth determines which of the 3 targets are being irradiated. The beam energy at front of target foil was determined on several occasions: 7.8 ± 0.1 MeV by a 2 copper-foil sandwich method (adopted from [3]). The available beam inside the cyclotron at extractor position is > 50 μA, and 35 μA are easily and long term reliably extracted (> 90 %) on to any of the 3 target positions. The prototype is capable of delivering more than 40 μA to target, but target current was limited to 35 μA under present unshielded conditions. Results 18F We have tested the prototype gridded (> 80 % transmission) niobium body target with 10μm Havar foil using 95 % 18O water and 35 μA on target + grid with yields given in TABLE 1. The observed yields corrected for stopping in foil, grid loss and water enrichment are 75 % of theoretical. One Fastlab FDG run using 2 h irradiation yielded 16 GBq FDG EOS, confirming the “usual” 18F activity. Results 11C Using gridded target and a 10μm foil with 99% N2 + 1 % O2 at 10 bar followed by trapping into ascarite gave EOB activity as shown in TABLE 2. Results 13N We know that the 16O(p,alpha)13N cross section is a very steep function of energy around 7.8 MeV. In the hope of using the simple water target route to 13N NH3 we have measured the 13N yields (corrected for 18F contribution). It is still unclear if these yields can be improved to make useful single doses of ammonia. Results for other isotopes We have used solid targets to make 45Ti, 64Cu, 68Ga and 89Zr. The development of these solid targets is still in progress, but especially the 68Ga yield looks promising (3 GBq EOB after 1 h on natural Zn will give > 15 GBq on enriched 68Zn).

A novel analytical method is developed to examine the chemical composition of plant oils by electrospray ionisation high-resolution Fourier transform ion cyclotron resonance mass spectrometry in both positive- and negative-ion modes. To date, this is the first reported application of this technique for the study of macadamia nut oil. Samples of macadamia nut oil from the Macadamia Integrifolia- Proteaceae family (smooth shell) are examined. The fatty acid profile of the oil is obtained by this mass spectrometric examination of the transesterified and hydrolysed oil samples. The Fourier transform ion-cyclotron resonance mass spectrometry results are compared to those obtained from similar samples using gas chromatography-mass spectrometry techniques. High performance liquid chromatography and Fourier transform ion cyclotron resonance mass spectrometry are used to separate and assign the isomers present in the methanol extract of the oils in separate experiments. Significant results in this study include: - The first observation and identity of a number of oxidised triacylglycerols in macadamia oil samples. - The first observation of oxidised and free fatty acids, measured directly in hydrolysed oil and in the methanol extract of macadamia oil. - High resolution Fourier transform ion cyclotron resonance mass spectrometry in broadband mode which enables isobars to be observed. - Esterified oil Fourier transform ion cyclotron resonance mass spectrometry results are consistent with our gas chromatography-mass spectrometry results and with the results of similar studies on macadamia oil in the literature. - A number of fatty acids with odd number of carbon atoms are observed in the oil. - In electrospray ionisation Fourier transform ion cyclotron resonance mass spectrometry of oils, the sample preparation is straightforward. The sample is dissolved in methanol or acetonitrile and the solution is introduced to the electrospray source directly. Introducing oil samples to the gas chromatograph-mass spectrometer needs the oils to be esterified prior to the analysis. - In this work, state-of-the-art mass spectrometry demonstrates distinct advantages in comparison to gas chromatography measurements such as direct identification of free fatty acids in oil samples, whereas this is not possible in gas chromatography-mass spectrometry due to the required esterification step prior to the analysis. - High performance liquid chromatography fraction collection is combined with Fourier transform ion cyclotron resonance mass spectrometry in off-line mode and found to improve the sensitivity, selectivity and signal to noise levels due to the lower number of compounds in each high performance liquid chromatography fraction compared to the methanol extract of macadamia oil sample. Also isomers of monoacylglycerols have been resolved using the high performance liquid chromatography technique.

Thesis (Ph. D.)--University of Adelaide, Dept. of Organic Chemistry, 1985. / Includes bibliographical references (leaves 177-193).

Thesis (Ph.D.)--McMaster University (Canada), 1995. / Source: Dissertation Abstracts International, Volume: 57-03, Section: B, page: 1870. Adviser: D. A. Thompson.