(3)He-particle-induced reactions on (nat)Sb for production of (124)I.

Excitation functions of the reactions (nat)Sb((3)He,xn)(124,123,121)I were measured from their respective thresholds up to 35 MeV, with particular emphasis on data for the production of the medically important radionuclide (124)I. The conventional stacked-foil technique was used. From the experimental data the theoretical yields of the three investigated radionuclides were calculated. The yield of (124)I over the energy range E9(30He) = 35 --> 13 MeV amounts to 0.95 MBq/microA h. The radionuclidic impurities are discussed. A comparison of (3)He- and alpha-particle-induced reactions on antimony for production of (124)I is given. The alpha-particle-induced reaction on enriched (121)Sb and the (3)He-particle-induced reaction on enriched (123)Sb would lead to comparable (124)I yields, but the level of impurities in the latter case would be somewhat higher.     

Excitation functions of (alpha,xn) reactions on (nat)Rb and (nat)Sr from threshold up to 26 MeV: possibility of production of (87)Y, (88)Y and (89)Zr.

Excitation functions were measured by the stacked-foil technique for (nat)Rb(alpha,xn)(87m,87m+g,88)Y and (nat)Sr(alpha,xn)(86,88,89)Zr reactions from their respective thresholds up to 26 MeV. The samples for irradiation were prepared by sedimentation and pellet pressing techniques. The measured data were compared with those available in the literature. From the excitation functions, integral yields of the products were calculated. The suitable energy ranges for the production of (87)Y and (88)Y via (nat)Rb(alpha,xn) processes and of (89)Zr via the (nat)Sr(alpha,xn) process are E(alpha)=26-->20 MeV, E(alpha)=26-->5 MeV and E(alpha)=20-->8.5 MeV, respectively. The respective yields amount to 8.2, 0.08 and 0.9 MBq/microA h. Production of (88)Y is feasible if a waiting time of about 2 months is allowed to let the impurities decay out. Also, (87)Y can be produced with a relatively low impurity of (88)Y. The yields of both (88)Y and (87)Y via the present routes are, however, appreciably lower than those via the (nat)Sr(p,xn) processes. There is a possibility to produce (89)Zr via the alpha-particle irradiation of (nat)Sr. The yield is rather low but would be considerably increased if enriched (86)Sr would be used as target material. The radionuclidic impurity levels in all the three products are discussed.     

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.     

Excitation functions of 124Te(d,xn)124,125I reactions from threshold up to 14 MeV: comparative evaluation of nuclear routes for the production of 124I.

Excitation functions of the nuclear reactions 124Te(d,xn)124-125I were measured from their respective thresholds up to 14.0 MeV via the stacked-foil technique. Thin samples were prepared by electrolytic deposition of 99.8% enriched 124Te on Ti-backing. The excitation function of the 124Te(d,n)125I reaction was measured for the first time. The present data for the 124Te(d,2n)124I reaction are by an order of magnitude higher than the literature experimental data but are in good agreement with the results of a hybrid model calculation. From the measured cross sections, integral yields of 124,125I were calculated. The energy range Ed = 14 --> 10 MeV appears to be the best compromise between 124I-yield and 1251-impurity. The calculated 124I-yield amounts to 17.5 MBq/microA h and the 125I-impurity to 1.7%. A critical evaluation of the three nuclear routes for the production of 124I, viz. 124Te(d,2n)-, 124Te(p,n)- and 125Te(p,2n)-processes, is given. The reaction studied in this work proved to be least suitable. The 124Te(p,n)-reaction gives 124I of the highest radionuclidic purity, and a small-sized cyclotron is adequate for production purposes. The 125Te(p,2n)-reaction is more suitable at a medium-sized cyclotron: the yield of 124I is four times higher than in the other two reactions but the level of 0.9% 125I-impurity is relatively high.     

Optimization of 124I production via 124Te(p,n)124I reaction.

(124)I was produced, via (124)Te(p,n)(124)I reaction, in greater than 3.7GBq (100 mCi, EOB) amount by bombarding (124)TeO(2) targets at 24 microA current for about 8h. This was achieved by keeping the target at 37 degrees relative to the beam during irradiation, by sweeping the beam across the target and by keeping the incident energy of the proton at 14.1MeV. The time-averaged yield of our 8h run was 21.1 MBq/microAh (0.57 mCi/microAh), which was 90% of the theoretical yield calculated using thick target yield data obtained from the reported excitation function for the reaction. At the end of bombardment, the level of (125)I and (126)I impurities, co-produced with (124)I, were 0.03% and 0.007%, respectively.     

Activation cross sections of the 169Tm(d,2n) reaction for production of the therapeutic radionuclide 169Yb.

Activation cross sections of deuteron induced nuclear reactions on (169)Tm were measured up to 20 MeV by using the stacked-foil technique. Special emphasis was on production of the internal radiotherapy related radionuclide (169)Yb. No earlier experimental cross-section data on deuteron induced reactions on (169)Tm were found in the literature. The experimental data were compared with the results of the nuclear model codes ALICE-IPPE and EMPIRE-II. The integral yield of the (169)Tm(d,2n)(169)Yb reaction was deduced over the optimum energy range Ed = 20-->9 MeV. At 3.8 MBq/microA.h the yield is lower than that available from the commonly used (168)Yb(n,gamma) (169)Yb reactor method but on the other hand, it is higher than the yields from the earlier investigated (169)Tm(p,n)(169)Yb and (nat)Er(alpha,x) (169)Yb reactions.     

Remote control production of an aqueous solution of no-carrier-added 34mCl- via the 32S(alpha,pn) nuclear reaction.

A remote system was established for the production of a biologically important radionuclide, chlorine-34m (32.0min, beta(+) 53%, IT 47%). The (32)S(alpha,pn)(34m)Cl reaction on elemental sulfur of natural isotopic composition was adopted for the production method. The target sulfur was melted by heating in the target chamber and then irradiated with 65MeV alpha particles (58.2MeV on target) at 3 microA for 30min. Generated (34m)Cl was extracted remotely with hot water from the molten sulfur in the target chamber. Within 20min, [(34m)Cl]chloride was obtained as a 10+/-3mL aqueous solution at a yield of 450 +/- 90 MBq, which corresponds to a recovery efficiency of 79 +/- 17% (n = 5). Both radionuclidic and radiochemical purities were more than 99% with a specific activity of 1.1GBq/ micromol. Non-radioactive impurities in the solution were identified as F(-), Cl(-), NO(3)(-), SO(4)(2-); other unknown ions were also present.     

Production of the therapeutic radionuclides 193mPt and 195mPt with high specific activity via alpha-particle-induced reactions on 192Os.

For the production of therapy-relevant radionuclides (193m)Pt (T(1/2)=4.33 d) and (195m)Pt (T(1/2)=4.03 d) with a high specific activity, the (192)Os(alpha,n)(195m)Pt and (192)Os(alpha,3n)(193m)Pt nuclear reactions were investigated for the first time from their respective thresholds up to 28 MeV. Thin samples of enriched (192)Os were prepared by electrodeposition on Ni, and the conventional stacked-foil technique was used for cross-section measurements. The calculated thick target yields were found to be 0.013 MBq/microA h for the (192)Os(alpha,n)(195m)Pt reaction in the energy range of E(alpha)=24-->18 MeV, and 0.25 MBq/microA h for the (192)Os(alpha,3n)(193m)Pt reaction in the energy range of E(alpha)=28-->24 MeV. The two radionuclides could not be detected in the interactions of (3)He particles with (192)Os. A production method involving high-current alpha-particle irradiation of enriched (192)Os and efficient chemical separation of radioplatinum was developed. Batch yields of about 1 MBq (195m)Pt and 8.7 MBq (193m)Pt were achieved. Compared to the reactor production these batch yields are very low, but the (192)Os(alpha,n)(195m)Pt and (192)Os(alpha,3n)(193m)Pt reactions are superior with respect to the specific activity of the products which is higher by two orders of magnitude.     

Experimental studies and nuclear model calculations on proton-induced reactions on Se, Se and Se with particular reference to the production of the medically interesting radionuclides Br and Br

Excitation functions of the reactions ^natSe(p,x)^75,76,77,82Br, ⁷⁶Se(p,xn)^75,76Br, ⁷⁶Se(p,x)⁷⁵Se and ⁷⁷Se(p,xn)^76,77Br were measured from their respective thresholds up to 40 MeV, with particular emphasis on data for the production of the medically important radionuclides ⁷⁶Br and ⁷⁷Br. The conventional stacked-foil technique was used. The samples were prepared by a sedimentation process. Irradiations were performed using the compact cyclotron CV 28 and the injector of COSY, both at the Research Centre Jülich. In order to validate the data, nuclear model calculations were performed using the code ALICE-IPPE which is based on the preequilibrium-evaporation model. Good agreement was found between the experimental and theoretical data, except in the high-energy region where the calculated data were somewhat higher. All the measured excitation curves were compared with the data available in the literature. From the experimental data the theoretical yields of all the investigated radionuclides were calculated and plotted as a function of proton energy. The calculated yield of ⁷⁷Br from the ^natSe(p,x)⁷⁷Br process over the energy range E_p=25→15 is 72.7 MBq/μA h and from the ⁷⁷Se(p,n)⁷⁷Br reaction over E_p=15→6 MeV it is 86.2 MBq/μA h. The yield of ⁷⁶Br from the ⁷⁶Se(p,n)⁷⁶Br reaction for E_p=15→8 is 360.1 MBq/μA h and from the ⁷⁷Se(p,2n)⁷⁶Br reaction for E_p=28→18 MeV it is 879.2 MBq/μA h. The radionuclidic impurity levels are discussed.     

Some optimisation studies relevant to the production of high-purity 124I and 120gI at a small-sized cyclotron.

Optimisation experiments on the production of the positron emitting radionuclides 124I(T(1/2) = 4.18d) and (120g)I (T(1/2) = 1.35 h) were carried out. The TeO(2)-target technology and dry distillation method of radioiodine separation were used. The removal of radioiodine was studied as a function of time and the loss of TeO(2) from the target as a function of oven temperature and time of distillation. A distillation time of 15 min at 750 degrees C was found to be ideal. Using a very pure source and comparing the intensities of the annihilation and X-ray radiation, a value of 22.0 +/- 0.5% for the beta(+) branching in 124I was obtained. Production of 124I was done using 200 mg/cm(2) targets of 99.8% enriched 124TeO(2) on Pt-backing, 16 MeV proton beam intensities of 10 microA, and irradiation times of about 8 h. The average yield of 124I at EOB was 470 MBq(12.7 mCi). At the time of application (about 70 h after EOB) the radionuclidic impurity 123I (T(1/2) = 13.2 h) was <1%. The levels of other impurities were negligible (126I < 0.0001%;125I = 0.01%). Special care was taken to determine the 125I impurity. For the production of (120g)I only a thin 30 mg target (on 0.5 cm(2) area) of 99.9% enriched 120TeO(2) was available. Irradiations were done with 16 MeV protons for 80 min at beam currents of 7 microA. The 120gI yield achieved at EOB was 700 MBq(19 mCi), and the only impurity detected was the isomeric state 120 mI(T(1/2) = 53 min) at a level of 4.0%. The radiochemical purity of both 124I and 120gI was checked via HPLC and TLC. The radioiodine collected in 0.02 M NaOH solution existed >98% as iodide. The amount of inactive Te found in radioiodine was <1 microg. High purity 124I and 120gI can thus be advantageously produced on a medium scale using the low-energy (p,n) reaction at a small-sized cyclotron.     

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.     

Radioiodination of 1-(2-deoxy-beta-D-ribofuranosyl)-2,4-difluoro-5-iodobenzene (dRFIB), a putative thymidine mimic nucleoside for cell proliferation studies

Iodine-124 was produced via the (124)Te(p,n)(124)I reaction by 15 MeV proton irradiation of an in-house solid mass tellurium dioxide target, using the Tübingen PETtrace (General Electric Medical Systems) cyclotron. 1-(2-Deoxy-beta-D-ribofuranosyl)-2,4-difluoro-5-iodobenzene (dRFIB), a stable, non-polar thymidine mimic nucleoside, was synthesized in 5 steps following a literature method, for radioiodination with [(124)I] iodide via isotope exchange in the presence of copper sulphate and ammonium sulphate in methanol-water. The radiolabelling procedure was optimized with respect to temperature, amount of dRFIB, amount of sodium hydroxide and reaction time, to produce radiochemical yields of up to 85% with a 1-h reaction at 140 degrees C. With routine I-124 production of 30 MBq/run, relatively high specific activities, approaching 100 MBq/mmol, can be expected. The activation energy for dRFIB radioiodination was calculated from temperature-time RCY data to be approximately 100 kJ/mol using no-carrier-added [(124)I]iodide.     

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.     

Comments on the feasibility of 61Cu production by proton irradiation of (nat)Zn on a medical cyclotron.

Feasibility of 61Cu production in high radionuclidic purity form via (nat)Zn(p,x) 61Cu nuclear process is discussed. Based on the experimentally available cross-sections of the (nat)Zn(p,x) 61Cu, (nat)Zn(p,x) 60Cu and (nat)Zn(p,x) 64Cu nuclear processes the usefulness of the (nat)Zn(p,x) 61Cu process for high-scale production is questionable in the 22 --> 12 MeV energy range.     

Cross sections of natSb(p,x) reactions for 30–46 MeV protons

In order to optimize the production of ¹¹⁸Te in thick targets for use in a ¹¹⁸Te/¹¹⁸Sb radionuclide generator, the excitation function for the ¹²¹Sb(p,4n)¹¹⁸Te reaction has been measured for 30–46 MeV protons. The excitation functions for the competing reactions ^natSb(p,xn)^119mTe, ^natSb(p,xn)¹¹⁹Te, ^natSb(p,xn)^121mTe, ^natSb(p,pxn)^120mSb and ¹²³Sb(p,pn)¹²²Sb have also been determined using stacked foil techniques. The ¹²¹Sb(p,4n)¹¹⁸Te reaction cross section maximum was found to be 480 mbarn at 44 MeV. In order to minimize the ^{119m + 119}Te interference a minimum proton beam energy of 40 MeV is required. The cross section results are compared with published data and with calculated excitation functions.     

A new binary compound for the production of 124I via the 124Te(p,n)124I reaction.

The binary compound, aluminum telluride (Al(2)Te(3)), was investigated as a target material for the production of (124)I by way of the (124)Te(p,n)(124)I reaction on a low-energy cyclotron. The high melting point and formation of a glassy matrix upon heating provided a stable target material at irradiations up to 20 microA of 11 MeV protons. The 87% tellurium mass fraction and 95% iodine separation yield led to significantly higher quantities of iodine compared to traditional TeO(2)/6%Al(2)O(3) admixtures. Radiochemical analysis of distilled samples using ion chromatography showed that the product remained in the iodide form while supported in weak buffer solutions. Stable Te impurities in the radioiodine product were less than 0.5 microg following purification by ion exchange chromatography. Average thick target yields of 229+/-18 microCi/microAh were achieved, and typical production runs at 18 microA for three hours yielded 12 mCi at the end-of-bombardment. Total losses of the target material after each irradiation and distillation cycle were approximately 2%.     

Experimental studies of the deuteron-induced activation cross-sections on natAg.

Excitation functions were measured for the (nat)Ag(d,x)(105,106m,110m)Ag, (nat)Ag(d,x)(107,109)Cd and (27)Al(d,x)(24)Na reactions by the stacked-foil activation technique and high-resolution gamma-spectroscopy over the energy range 0.44-40 MeV. The thick target integral yields were deduced using the measured cross-sections. No experimental data on the (nat)Ag+d process are available in the literature above 27 MeV. The nuclides (105)Ag, (106m)Ag and (109)Cd produced with deuteron induced activation of natural silver have suitable yields and decay characteristics important for thin layer activation (TLA) analysis. The cross-section for the production of (107)Cd and (109)Cd is significantly large. Therefore, the Ag+d process can be an efficient route for the production of isotope with a medium energy accelerator. The results of the model calculation using the TALYS code are not consistent with the present data. A large shift in the incident energy is found in TALYS calculations.     

Experimental study and nuclear model calculations on the 192Os(p,n)192Ir reaction: Comparison of reactor and cyclotron production of the therapeutic radionuclide 192Ir.

In a search for an alternative route of production of the important therapeutic radionuclide (192)Ir (T(1/2)=78.83 d), the excitation function of the reaction (192)Os(p,n)(192)Ir was investigated from its threshold up to 20 MeV. Thin samples of enriched (192)Os were obtained by electrodeposition on Ni, and the conventional stacked-foil technique was used for cross section measurements. The experimental data were compared with the results of theoretical calculations using the codes EMPIRE-II and ALICE-IPPE. Good agreement was found with EMPIRE-II, but slightly less with the ALICE-IPPE calculations. The theoretical thick target yield of (192)Ir over the energy range E(p)=16-->8 MeV amounts to only 0.16MBq/muA.h. A comparison of the reactor and cyclotron production methods is given. In terms of yield and radionuclidic purity of (192)Ir the reactor method appears to be superior; the only advantage of the cyclotron method could be the higher specific activity of the product.     

Excitation functions of proton-induced reactions on natFe and enriched 57Fe with particular reference to the production of 57Co

Excitation functions of the reactions ^natFe(p,xn)^55,56,57,58Co, ^natFe(p,x)⁵¹Cr, ^natFe(p,x)⁵⁴Mn, ⁵⁷Fe(p,n)⁵⁷Co and ⁵⁷Fe(p,α)⁵⁴Mn were measured from their respective thresholds up to 18.5 MeV, with particular emphasis on data for the production of the radionuclide ⁵⁷Co (T_1/2=271.8 d). The conventional stacked-foil technique was used, and the samples for irradiation were prepared by an electroplating or sedimentation process. The measured excitation curves were compared with the data available in the literature as well as with results of nuclear model calculations. From the experimental data, the theoretical yields of the investigated radionuclides were calculated as a function of the proton energy. Over the energy range E_p=15→5 MeV the calculated yield of ⁵⁷Co from the ⁵⁷Fe(p,n)⁵⁷Co process amounts to 1.2 MBq/μA h and from the ^natFe(p,xn)⁵⁷Co reaction to 0.025 MBq/μA h. The radionuclidic impurity levels are discussed. Use of highly enriched ⁵⁷Fe as target material would lead to formation of high-purity ⁵⁷Co.     

Experimental studies on excitation functions of the proton-induced activation reactions on yttrium.

Proton-induced activation cross-sections were measured for the (89)Y(p,x)(89,88,86)Zr, (89)Y(p,x)(88,87,87 m,86)Y, (89)Y(p,x)(85,83,82)Sr and (89)Y(p,x)(84,83)Rb reactions by a stacked foil technique in the energy range 15-80 MeV which was covered by two separate measurements for 15-50 and 32-80 MeV energy range with 50 and 80 MeV incident protons. The differences between the results of two irradiations were found within 6% in the overlapping energy regions. The production yields for the long-lived products like (88)Zr, and (88)Y are significantly larger than that of (nat)Mo+p, (nat)Nb+p and (nat)Zr+p processes. The productions of the medical isotopes, (85)Sr and (83)Sr are also effective by Y+p process using an 80 MeV beam. Thick target integral yields were also deduced using the measured cross-sections. The (87)Y, (88)Y, (88)Zr and (89)Zr radionuclides have suitable yields and decay characteristics important for thin-layer activation (TLA) analysis.