Separation of 44Ti from proton irradiated scandium by using solid-phase extraction chromatography and design of 44Ti/44Sc generator system.

Scandium-44g (half-life 3.97h [1]) shows promise for positron emission tomography (PET) imaging of longer biological processes than that of the current gold standard, 18F, due to its favorable decay parameters. One source of 44gSc is the long-lived parent nuclide 44Ti (half-life 60.0 a). A 44Ti/44gSc generator would have the ability to provide radionuclidically pure 44gSc on a daily basis. The production of 44Ti via the 45Sc(p,2n) reaction requires high proton beam currents and long irradiation times. Recovery and purification of no-carrier added (nca) 44Ti from scandium metal targets involves complex separation chemistry. In this study, separation systems based on solid phase extraction chromatography were investigated, including branched diglycolamide (BDGA) resin and hydroxamate based ZR resin. Results indicate that ZR resin in HCl media represents an effective 44Ti/44gSc separation system.

Large scale accelerator production of 225Ac: Effective cross sections for 78-192MeV protons incident on 232Th targets.

Actinium-225 and 213Bi have been used successfully in targeted alpha therapy (TAT) in preclinical and clinical research. This paper is a continuation of research activities aiming to expand the availability of 225Ac. The high-energy proton spallation reaction on natural thorium metal targets has been utilized to produce millicurie quantities of 225Ac. The results of sixteen irradiation experiments of thorium metal at beam energies between 78 and 192MeV are summarized in this work. Irradiations have been conducted at Brookhaven National Laboratory (BNL) and Los Alamos National Laboratory (LANL), while target dissolution and processing was carried out at Oak Ridge National Laboratory (ORNL). Excitation functions for actinium and thorium isotopes, as well as for some of the fission products, are presented. The cross sections for production of 225Ac range from 3.6 to 16.7mb in the incident proton energy range of 78-192MeV. Based on these data, production of curie quantities of 225Ac is possible by irradiating a 5.0gcm-2 232Th target for 10 days in either BNL or LANL proton irradiation facilities.

Application of ion exchange and extraction chromatography to the separation of actinium from proton-irradiated thorium metal for analytical purposes.

Actinium-225 (t1/2=9.92d) is an α-emitting radionuclide with nuclear properties well-suited for use in targeted alpha therapy (TAT), a powerful treatment method for malignant tumors. Actinium-225 can also be utilized as a generator for (213)Bi (t1/2 45.6 min), which is another valuable candidate for TAT. Actinium-225 can be produced via proton irradiation of thorium metal; however, long-lived (227)Ac (t1/2=21.8a, 99% ß(-), 1% α) is co-produced during this process and will impact the quality of the final product. Thus, accurate assays are needed to determine the (225)Ac/(227)Ac ratio, which is dependent on beam energy, irradiation time and target design. Accurate actinium assays, in turn, require efficient separation of actinium isotopes from both the Th matrix and highly radioactive activation by-products, especially radiolanthanides formed from proton-induced fission. In this study, we introduce a novel, selective chromatographic technique for the recovery and purification of actinium isotopes from irradiated Th matrices. A two-step sequence of cation exchange and extraction chromatography was implemented. Radiolanthanides were quantitatively removed from Ac, and no non-Ac radionuclidic impurities were detected in the final Ac fraction. An (225)Ac spike added prior to separation was recovered at ≥ 98%, and Ac decontamination from Th was found to be ≥ 10(6). The purified actinium fraction allowed for highly accurate (227)Ac determination at analytical scales, i.e., at (227)Ac activities of 1-100 kBq (27 nCi to 2.7 µCi).

Proton-induced cross sections relevant to production of 225Ac and 223Ra in natural thorium targets below 200 MeV.

Cross sections for (223,)(225)Ra, (225)Ac and (227)Th production by the proton bombardment of natural thorium targets were measured at proton energies below 200 MeV. Our measurements are in good agreement with previously published data and offer a complete excitation function for (223,)(225)Ra in the energy range above 90 MeV. Comparison of theoretical predictions with the experimental data shows reasonable-to-good agreement. Results indicate that accelerator-based production of (225)Ac and (223)Ra below 200 MeV is a viable production method.

225Ac and 223Ra production via 800 MeV proton irradiation of natural thorium targets.

Cross sections for the formation of (225,227)Ac, (223,225)Ra, and (227)Th via the proton bombardment of natural thorium targets were measured at a nominal proton energy of 800 MeV. No earlier experimental cross section data for the production of (223,225)Ra, (227)Ac and (227)Th by this method were found in the literature. A comparison of theoretical predictions with the experimental data shows agreement within a factor of two. Results indicate that accelerator-based production of (225)Ac and (223)Ra is a viable production method.

Radioarsenic from a portable (72)Se/(72)As generator: a current perspective.

Positron emission tomography (PET) of slower biological processes calls for the use of longer lived positron emitting radioisotopes. Beyond radionuclide production considerations, practicality and rapidity of subsequent labeling chemistry further limits the selection of radioisotopes with potentially favorable nuclear properties. One additional limitation is the availability of PET radiotracers at the point-of-care with appropriate on-site production methodologies or robust radionuclide generator systems. The positron emitter (72)As (half-life 26 h) is generated via decay of (72)Se (half-life 8.5 d); this pair comprises and excellent generator system for clinical availability of a longer lived PET isotope. Many (72)Se/As generator systems have been introduced utilizing the rich interplay of Se(IV)/Se(VI) and As(III) /As(V) chemical behavior. This paper describes available generator concepts, and briefly outlines some current arsenic labeling methodologies for the introduction of radioarsenic into biomolecules.

Selenium-72 formation via nat Br(p,x) induced by 100 MeV protons: steps towards a novel 72Se/72As generator system.

Selenium-72 production by the proton bombardment of a natural NaBr target has been successfully demonstrated at the Los Alamos National Laboratory Isotope Production Facility (LANL-IPF). Arsenic-72 (half life 26 h) is a medium-lived positron emitting radionuclide with the major advantage of being formed as the daughter of another "generator" radioisotope (Se-72, 8.5 d). A (72)Se/(72)As generator would be the preferred mechanism for clinical utilization of (72)As for positron emission tomography (PET). No portable (72)Se/(72)As generator system has been demonstrated for convenient, repeated (72)As elution ("milking"). In this work, we describe (72)Se production and recovery from irradiated NaBr targets using a 100 MeV proton beam. We also introduce an (72)As generator principle based on (72)Se chelation followed by liquid-liquid extraction, which will be transferred to a solid-phase sorption/elution system.

Excitation functions of natGe(p,xn)71,72,73,74 As reactions up to 100 MeV with a focus on the production of 72 As for medical and 73 As for environmental studies.

Excitation functions for the formation of the arsenic radionuclides (71)As, (72)As, (73)As and (74)As in the interaction of protons with (nat)Ge were measured from the respective threshold energy up to 100 MeV. The conventional stacked-foil technique was used and the needed thin samples were prepared by sedimentation. Irradiations were done at three cyclotrons: CV 28 and injector of COSY at Forschungszentrum Jülich, and Separate Sector Cyclotron at iThemba LABS, Somerset West. The radioactivity was measured via high-resolution gamma-ray spectrometry. The measured cross section data were compared with the literature data as well as with the nuclear model calculations. In both cases, the results generally agree but there are discrepancies in some areas, the results of nuclear model calculation and some of the literature data being somewhat higher than our data. The integral yields of the four radionuclides were calculated from the measured excitation functions. The beta(+) emitting nuclide (72)As (T(1/2)=26.01 h) can be produced with reasonable radionuclidic purity ((71)As impurity: <10%) over the energy range E(p) = 18-->8 MeV; the yield of 93 MBq/microAh is, however, low. The radionuclide (73)As (T(1/2)=80.30 d), a potentially useful indicator in environmental studies, could be produced with good radionuclidic purity ((74)As impurity: <11%) over the energy range E(p) = 30 --> 18 MeV, provided, a decay time of about 60 days is allowed. Its yield would then correspond to 2.4 MBq/microAh, and GBq amounts could be produced when using a high current target.

Excitation functions for the production of 82Sr by proton bombardment of natRb at energies up to 100 MeV.

The excitation functions for the production of (82)Sr and other radionuclides produced in the proton bombardment of rubidium were measured by means of the activation technique. Stacks were assembled from RbCl targets, aluminium and copper monitor foils and bombarded with protons of energy up to 100 MeV and nominal current 0.1 microA. The measured data were compared with the theoretical calculations obtained by means of ALICE-IPPE, and also with previously published data. The measured data sets exhibit good agreement at incident energies below 45 MeV and greater than 60 MeV but show large discrepancies in the energy range between these values. The ALICE-IPPE calculations evidently overestimate all reported experimental cross sections, in particular overestimating the present data by a factor of 1.6. Notwithstanding the fact that there are discrepancies in the cross sections, good agreement is found with regards to the shape of the excitation function.

Excitation functions of 85Rb(p,xn)(85m,g,83,82,81)Sr reactions up to 100 MeV: integral tests of cross section data, comparison of production routes of 83Sr and thick target yield of 82Sr.

The beta+ emitter 83Sr (T(1/2) = 32.4 h, Ebeta+ = 1.23 MeV, Ibeta+ = 24%) is a potentially useful radionuclide for therapy planning prior to the use of the beta+ emitter 89Sr (T(1/2) = 50.5 d). In order to investigate its production possibility, cross section measurements on the 85Rb(p,xn)-reactions, leading to the formation of the isotopes (85m,g)Sr, 83Sr, 82Sr and 81Sr, were carried out using the stacked-foil technique. In a few cases, the products were separated via high-performance liquid chromatography. For 82Sr, both gamma-ray and X-ray spectrometry were applied; in other cases only gamma-ray spectrometry was used. From the measured excitation functions, the expected yields were calculated. For the energy range Ep = 37 --> 30 MeV the 83Sr yield amounts to 160 MBq/microA h and the level of the 85gSr (T(1,2) = 64.9 d) and 82Sr (T(1/2) = 25.5 d) impurities to <0.25%. In integral tests involving yield measurements radiostrontium was chemically separated and its radioactivity determined. The experimental production data agreed within 10% with those deduced from the excitation functions. The results of the 85Rb(p,3n)83Sr reaction were compared with the data on the production of 83Sr via the 82Kr(3He,2n)-process. In the energy range E3Hc = 18 --> 10 MeV the theoretical yield of 83Sr amounts to 5 MBq/microA h and the 82Sr impurity to about 0.2%. The method of choice for the production of 83Sr is thus the 85Rb(p,3n)-process, provided a 40 MeV cyclotron is available. During this study some supplementary information on the yield and purity of 82Sr was also obtained.

Excitation functions of 125Te(p, xn)-reactions from their respective thresholds up to 100 MeV with special reference to the production of 124I.

Excitation functions of the nuclear reactions 125Te(p, xn) (119,120m, 120g, 121,122,123,124,125)I were measured for the first time from their respective thresholds up to 100 MeV using the stacked-foil technique. Thin samples were prepared by electrolytic deposition of 98.3% enriched 125Te on Ti-backing. In addition to experimental studies, excitation functions were calculated by the modified hybrid model code ALICE-IPPE. The experimental and theoretical data generally showed good agreement. From the measured cross section data, integral yields of (123,124,125)I were calculated. The energy range Ep 21 --> 15 MeV appears to be very suitable for the production of the medically interesting radionuclide 124I (T(1/2) = 4.18 d; I(beta)+ = 25%). The thick target yield of 124I amounts to 81 MBq/microA h and the level of 125I-impurity to 0.9%. The 125Te(p,2n)124I reaction gives 124I yield about four times higher than the commonly used 124Te(p,n)124I and 124Te(d,2n)124I reactions. The proposed production energy range is too high for small cyclotrons but large quantities of 124I can be produced with medium-sized commercial machines.

Integral excitation functions for natKr + p up to 116 MeV and optimization of the production of 81Rb for (81m)Kr generators.

Effective cross-sections for the production of 79,81,81m,82m,83,84,84m,86Rb, (77,79,85m)Kr and 77,82Br in the bombardment of natKr with protons were measured from threshold up to 116 MeV. Thick-target production-rate curves based on the measured integral excitation functions were also derived for 81,82m,83,84,86Rb, and the optimum incident energy for the production of 81Rb/(81m)Kr, as a function of the target thickness in MeV, was determined. Geometry-dependent hybrid-model calculations performed by means of the computer code ALICE/85/300 were found to be in good agreement with the experimental results as well as the derived thick-target production-rate curves.

Production of 52Fe via proton-induced reactions on manganese and nickel.

Excitation functions for the production of 52Fe in the bombardment of Mn and Ni with protons were measured from threshold up to 200 MeV. Production rates of 52Fe as well as of its 55Fe and 59Fe impurities were also measured in specific energy windows ranging up to 100 MeV. The agreement with previous measurements, where available, is reasonably good, except that considerably higher 55Fe contamination levels than those recently reported below 70 MeV were obtained in the case of Ni. The experimental results were compared with theoretical calculations by means of the computer code ALICE/85/300. Overall agreement to within a factor of two was obtained, and the usefulness of the code in planning a radioisotope production process was demonstrated. Finally, practical production rates and impurity levels, obtained with a 66 MeV proton beam at high intensities (approximately 50 microA), are reported.