New cross section data on68Zn(p, 2n)67Ga andnatZn(p,xn)67Ga nuclear reactions for the development of a reference data base

Excitation functions were measured by stacked-foil technique for the⁶⁸Zn(p, 2n)⁶⁷Ga,⁶⁸Zn(p,3n)⁶⁶Ga,^natCu(p,xn)⁶²Zn,^natZn(p,xn)⁶⁷Ga,^natZn(p,xn)⁶⁶Ga,^natZn(p,px)⁶²Zn and^natZn(p,αx)⁶¹Cu nuclear reactions in the energy range from 15–35 MeV. The experimental excitation functions were compared with published data. Our present measurements not only increase the number of available cross section data points for the above reactions, but for some reactions (and in some energy regions) values are presented for the first time.     

Nuclear model calculation for cyclotron production of 61Cu as a PET imaging

⁶¹Cu is positron emitter and can be used as the PET and molecular imaging. In this study cyclotron production of ⁶¹Cu via ⁶¹Ni(p,n)⁶¹Cu, ^natNi(p,x)⁶¹Cu, ^natNi(d,x)⁶¹Cu, ^natNi(α,x)⁶¹Cu, ^natZn(p,x)⁶¹Cu and ⁵⁹Co(α,2n)⁶¹Cu reactions was investigated. The ALICE/ASH (hybrid and GDH models) and TALYS-1.2 codes were used to calculate excitation functions for proton, alpha and deuteron induced on ^natNi, proton on ⁶¹Ni and ^natZn and also alpha-particle on ⁵⁹Co targets that lead to the production of ⁶¹Cu radioisotopes using intermediate energy accelerators. In addition, we compared the data obtained from in this study with the reported measurement by experimental data. Moreover, optimal thickness of the targets and physical yield were obtained by stopping and range of ions in matter code for each reaction. Eventually ⁶¹Ni(p,n)⁶¹Cu and ⁵⁹Co(α,2n)⁶¹Cu reaction to produce ⁶¹Cu in no-carrier added state with high production yield was suggested. Finally the ^natNi(p,x)⁶¹Cu reaction was employed to test the target preparation using electroplating technique.     

Targetry and specification of <Superscript>167</Superscript>Tm production parameters by different reactions

In recent years, there has been a rapid expansion in the use of radio nuclides for therapeutic purposes. Thulium–167 is an important radionuclide (T _1/2 = 9.25 d) due to it could be used for tumor and bone studies in nuclear medicine. ¹⁶⁷Tm complexed with hydroxy ethylene diamine tetra-acetic acid (HEDTA) could be used with the aim of bone imaging. ¹⁶⁷Tm emits a prominent γ ray of 208 keV energy and low energy electrons. This study describes calculations on the excitation functions of ¹⁶⁵Ho(α,2n)¹⁶⁷Tm, ¹⁶⁷Er(p,n)¹⁶⁷Tm, ^natEr(d,xn)¹⁶⁷Tm and ^natEr(p,xn)¹⁶⁷Tm reactions by ALICE/ASH (hybrid and GDH models) and TALYS-1.0 codes. In addition, calculated data by codes were compared to experimental data that earlier were published and TENDL-2010 database. Moreover, optimal thickness of the targets and physical yield were obtained by SRIM (stopping and range of ions in matter) code for each reaction. According to the results, the ¹⁶⁷Er(p,n)¹⁶⁷Tm and ¹⁶⁵Ho(α,2n)¹⁶⁷Tm reactions are suggested as the best method to produce ¹⁶⁷Tm owing to minimum impurities. The TALYS-1.0 code, predict the maximum cross-section of about 382 mb at 11 MeV and 849 mb at 26 MeV for ¹⁶⁷Er(p,n)¹⁶⁷Tm and ¹⁶⁵Ho(α,2n)¹⁶⁷Tm reactions, respectively. Finally, deposition of ^natEr₂O₃ on Cu substrate was carried out via the sedimentation method. The 516 mg of erbium(III)oxide with 103.2 mg of ethyl cellulose and 8 mL of acetone were used to prepare a ^natEr₂O₃ layer of 11.69 cm². ¹⁶⁷Tm was produced via the ^natEr(p,n)¹⁶⁷Tm nuclear process at 20 μA current and 15 → 7 MeV protons beam (1 h). Yield of about 3.2 MBq ¹⁶⁷Tm per μA h were experimentally obtained.     

Development of [<Superscript>64</Superscript>Cu]-DOTA-anti-CD20 for targeted therapy

Copper-64 was produced as a by-product of ⁵⁵Co via ⁶⁴Ni(p,n)⁶⁴Cu by 15 MeV proton bombardment of ^natNi resulting in a thick target yield of 5.31 MBq/μAh (143.5 μCi/μAh) and a radiochemical separation yield of 95% (radionuclide purity >97% after 25 hours of bombardment). Rituximab was successively labeled with [⁶⁴Cu]-CuCl₂. N-succinimidyl-1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA-NHS) was prepared at 25 °C using DOTA and N-hydroxy succinimide (NHS) in CH₂Cl₂ followed by the addition of 1 ml of a Rituximab pharmaceutical solution. Radiolabeling was performed at 37 °C in 3 hours. Radio thin-layer chromatography showed an overall radiochemical purity of 90–95% at optimized conditions (specific activity=30 GBq/mg, labeling efficacy; 82%) using various chromatography systems. The final isotonic ⁶⁴Cu-DOTA-Rituximab complex was passed through a 0.22 μm filter and checked by gel electrophoresis for radiolysis control. Stability of the final product was checked in the formulation and in presence of human serum at 37 °C.     

Radiochemical separation and quality assessment for the <Superscript>68</Superscript>Zn target based <Superscript>64</Superscript>Cu radioisotope production

The radiochemical separation of the different radionuclides (⁶⁴Cu, ⁶⁷Cu, ⁶⁷Ga, ⁶⁶Ga, ⁵⁶Ni, ⁵⁷Ni, ⁵⁵Co, ⁵⁶Co, ⁵⁷Co, ⁶⁵Zn, ¹⁹⁶Au) induced in the Ni supported Cu substrate — ⁶⁸Zn target system, which was bombarded with the 29.0 MeV proton beam, was performed by ion-exchange chromatography using successive isocratic and/or concentration gradient elution techniques. The overlapped gamma-ray spectrum analysis method was developed to assess the ⁶⁷Ga and ⁶⁷Cu content in the ⁶⁴Cu product and even in the post-⁶⁷Ga production ⁶⁸Zn target solution without the support of radiochemical separation. This method was used for the assessment of ⁶⁴⁺⁶⁷Cu radioisotope separation from ⁶⁷Ga, the quality control of ⁶⁴Cu product and the determination of the ⁶⁸Zn (p,2p)⁶⁷Cu reaction yield. The improvement in the targetry and the optimization of proton beam energy for the ⁶⁸Zn target based ⁶⁴Cu and ⁶⁷Ga production were proposed based on the stopping power and range of the incident proton and on the excitation functions, reaction yields and different radionuclides induced in the target system.     

Production and chemical separation of <Superscript>48</Superscript>V

Summary Vanadium-48 was produced with an activity of 222 MBq (6 mCi) by the ^natTi(d,xn)⁴⁸V nuclear reactions in the U-120 cyclotron. The energy of the irradiating beam was 13 MeV, its intensity 5 μA, and the metallic Ti target dimension 11’11 mm² (0.1 mm thickness). For target cooling, circulated water in target backside was used. After 3 cooling days, only ⁴⁸V and some ⁴⁶Sc (T_1/2 = 83.8 d), produced by the side nuclear reaction ⁴⁸Ti(d,α)⁴⁶Sc were found in the target. For production of the radiotracer of ⁴⁸V and for the preparation of source for standardization of ⁴⁸V by 4πβ-γ coincidence, the Ti target was dissolved either in HF or in H₂SO₄. For both dissolving methods an ion-exchange separation procedure was developed.     

Optimization of the production of [61Cu]Diacetyl-bis(N 4-methylthiosemicarbazone) for PET studies

Summary Copper-61 produced via the ^natZn(p,x)⁶¹Cu nuclear reaction was used for the preparation of [⁶¹Cu]diacetyl-bis(N⁴-methylthiosemicarbazone) ([⁶¹Cu]ATSM) (4) using a house-made ATSM ligand. After a proton irradiation of an electroplated zinc layer by 22 MeV protons at 180 mA for 3.2 hours, ⁶¹Cu was recovered by two-step chromatography using a cation and an anion exchange column. About 222 GBq (6.00 Ci) of ⁶¹Cu²⁺ was obtained with a radiochemical separation yield of more than 95% and a radionuclidic purity of better than 99%. Colorimetric methods showed that traces of chemical impurities in the product were below the accepted limits. The [⁶¹Cu]ATSM production was optimized for reaction conditions (buffer concentration and temperature) with a radiochemical yield of higher than 80%, radiochemical purity of better than 98% and a specific activity of about 246 Ci/mmol. The produced [⁶¹Cu]ATSM is a PET radiotracer for hypoxia imaging with an intermediate half life and a satisfactory quality, suitable for future PET studies.     

Study of the cyclotron production of <Superscript>172</Superscript>Lu: an excellent radiotracer

¹⁷²Lu due to its suitable (T _1/2 = 6.7 days) and high detection sensitivity, is used as a radiotracer in different fields. ¹⁷²Lu appears to be suitable as a long-lived rare-earth tracer for compound labelling and biodistribution studies. In the present study, excitation functions via ¹⁷²Yb(p,n)¹⁷²Lu, ^natYb(p,xn)¹⁷²Lu, ¹⁷²Yb(d,2n)¹⁷²Lu and ^natYb(d,xn)¹⁷²Lu reactions were calculated by ALICE/91, ALICE/ASH and TALYS-1.2 codes. Deposition of ^natYb₂O₃ on Cu substrate was carried out via sedimentation method for the production of ¹⁷²Lu. Cementation separation process and liquid–liquid extraction (LLX) of no-carrier-added (nca) radiolutetium from irradiated ytterbium(III)oxide target hydrochloric solution was described using Na(Hg) amalgam, α-hydroxyisobutyric acid (α-HIB) and di-(2-ethylhexyl)phosphoric acid (HDEHP).     

Production of <Superscript>122</Superscript>Sb for the study of environmental pollution

This article presents, ¹²²Sb (T _1/2 = 2.723 days, I _β- = 97.59%) was produced via the ^natSn(p,xn) nuclear process at the AMIRS (Cyclone-30, IBA, Belgium). The electrodeposition experiments were carried out by potassium stannate trihydrate (K₂Sn(OH)₆) and potassium hydroxide. The optimum conditions of the electrodeposition of tin were as follows: 40 g/L ^natSn, 20 g/L KOH, 115 g/L K₂Sn(OH)₆, DC current density of 5 A/dm² with a bath temperature of 75 °C. The electroplated Tin-target was irradiated with 26.5 MeV protons at current of 180 μA for 20 min. Solvent extraction of no-carrier-added ¹²²Sb from irradiated Tin-natural target hydrochloric solution was investigated using di-n-butyl ether (C₈H₁₈O). Yields of about 3.61 MBq/μAh were experimentally obtained.     

A comparative study on the separation of radioyttrium from Sr- and Rb-targets via ion-exchange and solvent extraction techniques,with special reference to the production of no-carrier-added <Superscript>86</Superscript>Y, <Superscript>87</Superscript>Y and <Superscript>88</Superscript>Y using a cyclotron

The radiochemical separation of ⁸⁸Y from proton irradiated ^natSrCO₃ and alpha-particle irradiated ^natRbCl, of ⁸⁶Y from proton irradiated ⁸⁶SrCO₃, and of ⁸⁷Y from alpha-particle irradiated ^natRbCl were studied at no-carrier-added levels by two techniques, namely, ion-exchange chromatography using Dowex 50W-X8 and Dowex 21K resins, and solvent extraction using HDEHP. Out of all those methods, the ion-exchange chromatography using Dowex 50W-X8 (cation-exchanger) was found to be the best: the separation yield was high, the chemical impurity in the separated radioyttrium (inactive Sr or Rb) was low (0.5 μg) and the final product was obtained in the form of citrate. The optimized separation method using Dowex 50W-X8 was applied in practical production of ⁸⁶Y and ⁸⁸Y via proton irradiations of ⁸⁶SrCO₃ and ^natSrCO₃, respectively, at 16 MeV as well as of ⁸⁷Y and ⁸⁸Y via α-particle irradiation of ^natRbCl at 26 MeV. The tangible experimental yields of ⁸⁶Y and ⁸⁷Y amounted to 150 and 5.7 MBq/μA·h, respectively. The yields of ⁸⁸Y obtained were 0.06 MBq/μA·h and 1 MBq/μA·h for alpha-particle and proton irradiations, respectively. Each yield value corresponds to more than 70% of the respective theoretical value.     

Measurement of activation cross sections of the proton induced nuclear reactions on palladium

Excitation functions of proton induced reactions on Pd are important for medical radioisotope production, for activation analysis, for development of low activation materials and other purposes. No experimental data exist in the literature for low and medium energy range protons. A detailed study of the excitation functions was performed up to 80 MeV proton energy by using the stacked foil irradiation technique and gamma-ray spectrometry. The irradiations were carried out at the external beam lines of the AVF cyclotron at the Tohoku University. Japan (80 and 70 MeV) and the CGR 560 cyclotron at the Vrije Universiteit Brussels (38, 29 and 17 MeV). The beam intensity, the incident energy and the energy degradation were controlled by a method based on flux constancy via normalization to the parallel measured excitation functions of ^natAl(p,x)^22,24Na and ^natCu(p,x)^56,58Co, ^62,65Zn monitor reactions. Excitation functions for direct and cumulative cross sections have been measured for the production of ^{105mg,106m,110m}Ag, ¹⁰¹Pd, ^101mRh and ⁹⁷Ru radionuclei. Calculations for the excitation functions using the Alice-IPPE code were performed with a view to estimate the weight of the different contributing reactions and to check the trend and the magnitude of the obtained experimental data.     

Experimental study and nuclear model calculation for 65Zn production

Excitation functions and theoretical yields via charge particle induced reactions were evaluated using EMPIRE-3.2.2 and ALICE/ASH codes and the obtained results have been discussed and compared with the available reported experimental data. It has been verified that ^natCu(p,n)⁶⁵Zn reaction is the optimum ⁶⁵Zn production route. The ⁶⁵Zn was produced using ^natCu(p,xn) ⁶⁵Zn reaction in the energy range of 16.8 → 12.2 MeV with the thick target yield of 0.15 ± 0.005 MBq/μA h. The ⁶⁵Zn radionuclide was purified by anion exchange chromatography.

     

Measurements of fast neutron capture cross sections on <Superscript>63</Superscript>Cu and <Superscript>186</Superscript>W

Neutron capture cross sections on ⁶³Cu and ¹⁸⁶W were measured by fast neutron activation method at neutron energies from 1 to 2 MeV. Monoenergetic fast neutrons were produced by ³H(p,n)³He reaction. Neutron energy spread by target thickness, which was assumed to be the main factor of neutron energy spread, was estimated to be 1.5% at neutron energy of 2.077 MeV. Neutron capture cross sections on ⁶³Cu and ¹⁸⁶W were calculated by reference comparison method on those of ¹⁹⁷Au(n,γ). Not only statistical errors of gamma-counts from samples but also systematic errors in the counting efficiency for HP Ge detector and the uncertainty of areal density of samples were considered in calculating neutron capture cross section. Estimated neutron capture cross sections on ⁶³Cu and ¹⁸⁶W were also compared with ENDF-6 data.     

Investigation of solution chemistry effects on sorption behavior of radionuclide <Superscript>64</Superscript>Cu(II) on illite

In this work, a series of batch experiments were carried out to investigate the effect of various environmental factors such as contact time, pH, ionic strength, coexisting electrolyte ions, humic substances and temperature on the sorption behavior of illite towards ⁶⁴Cu(II). The results indicated that ⁶⁴Cu(II) sorption on illite achieved equilibrium quickly. The pH- and ionic strength-dependent sorption suggested that ⁶⁴Cu(II) sorption on illite was dominated by ion exchange or outer-sphere surface complexation at pH < 7, whereas the pH-dependent and ionic strength-independent sorption indicated that the sorption process was mainly attributed to inner-sphere surface complexation at pH > 7. A positive effect of humic substances on ⁶⁴Cu(II) sorption was found at pH < 6.5, whereas a negative effect was observed at pH > 6.5. The Langmuir and Freundlich models were used to simulate the sorption isotherms of ⁶⁴Cu(II) at three different temperatures of 293, 313, and 333 K. The thermodynamic parameters (ΔH ⁰, ΔS ⁰, and ΔG ⁰) of ⁶⁴Cu(II) sorption on illite were calculated from the temperature dependent sorption isotherms, and the results indicated that the sorption of ⁶⁴Cu(II) on illite was endothermic and spontaneous. From the experimental results, it is possible to conclude that illite has good potentialities for cost-effective treatments of ⁶⁴Cu(II)-contaminated wastewaters.     

A novel technique for simultaneous diagnosis and radioprotection by radioactive cerium oxide nanoparticles: study of cyclotron production of <Superscript>137m</Superscript>Ce

Application of nanoparticles in nuclear medicine has aimed to develop diagnosis and therapeutic techniques. Cerium oxide nanoparticles (CNPs) are expected to be useful for protection of healthy tissue from radiation-induced harm and could serve therapeutic function. Among a variety of cerium radioisotopes, ^137mCe (T _1/2 = 34.4 h, IT (99.22%), β⁺ (0.779%)) could be a novel candidate radionuclide in the field of diagnosis owing to its appropriate half-life, 99.91% natural abundance of target and its intense gamma line at 254.29 keV. In this study, ^137mCe excitation function via the ^natLa(p,3n) reaction was calculated by TALYS-1.2 and EMPIRE-3 codes. The excitation function calculations demonstrated that the ^natLa(p,3n)^137mCe reaction leads to the formation of the ^136/138Ce isotopic contamination in the 22–35 MeV energy range. Interestingly, the isotopic impurities of ^137mCe could serve radio protector function. Overall results indicate that the cyclotron produced ^137mCeO₂ nanoparticles by irradiation of a target encompassing lanthanum oxide nanoparticles could be a potent alternative for conventional diagnostic radionuclides with simultaneous radioprotection capacity.     

Production of <Superscript>88,89</Superscript>Zr by proton induced activation of <Superscript>nat</Superscript>Y and separation by SLX and LLX

^natY foil was irradiated by 20 MeV proton to produce no-carrier-added ^88,89Zr. A comparative evaluation on radioanalytical separation methods of ^88,89Zr was carried out from irradiated target matrix by both liquid–liquid (LLX) and solid–liquid (SLX) extraction methods using di-(2-ethylhexyl) phosphoric acid (HDEHP) dissolved in cyclohexane as liquid cation exchanger and Dowex 50W-X8 H⁺ form (20–50 mesh) as solid cation exchanger. Both the methods offer good separation and high yield of nca ^88,89Zr but SLX offers much higher separation factor and better yield.     

Characterisation of a Cu selective resin and its application to the production of <Superscript>64</Superscript>Cu

Cu isotopes (e.g. ⁶⁴Cu) increasingly find use in radiopharmaceutical applications, accordingly fast and reliable methods for the production of these isotopes are needed. The aim of the presented project is the characterization of a Cu selective extraction chromatographic resin for the fast and selective separation of Cu radionuclides, e.g. from irradiated targets. The characterisation of the resin includes the determination of weight distribution factors D _w of Cu, Ni, Zn and other potentially interfering elements and impurities for varying acids and pH values, the influence of macro amounts of Ni and Zn on the extraction of Cu as well as the influence of other potential interferents. Based on the obtained results, a method for the separation of Cu and its purification from irradiated Ni or Zn targets was developed and tested on simulated Ni and Zn targets.     

Deuteron-induced activation cross-sections on natural copper up to 24 MeV

Activation cross-sections of ^natCu(d,x)^62,65Zn,⁶⁴Cu,^60g+mCo,⁵⁹Fe reactions were measured using a stacked foil activation technique combined with HPGe gamma-ray spectrometry up to the deuteron energy of 24 MeV. Measured data were critically compared with the available literature data and theoretical data extracted from the TENDL-2012 library, and found only partial agreements among them. Cross-sections of ^natCu(d,x)⁵⁹Fe reactions are reported here for the first time in the energy region of 19–23 MeV. Measured cross-sections of the long-lived ⁶⁵Zn, ^60gCo and ⁵⁹Fe radionuclides are significant for understanding the activation behaviour of copper, an essential structural material used in accelerator and nuclear industry.     

Migration processes of <Superscript>137</Superscript>Cs and <Superscript>90</Superscript>Sr in compartments of a lake ecosystem

Summary The dispersion of radioactive substances in the environment following nuclear weapon tests in atmosphere since 1954 and accidents to nuclear plants, like that in Chernobyl in 1986, have allowed us to study the migration processes of some radionuclides in complex ecosystems such as lakes are. In the present paper the behavior of ¹³⁷Cs and ⁹⁰Sr in different compartments of the Monterosi Lake (central Italy) was assessed. The ¹³⁷Cs concentration was measured in lake water as well as sediment, stream water, aquatic plant and fish samples. ⁹⁰Sr concentration in water and sediments was also determined. A total inventory of 4206±76 Bq ^. m^-2 and 958±79 Bq ^. m^-2 (on 27/6/01) has been found for ¹³⁷Cs and ⁹⁰Sr, respectively. The experimental data presented here allow to calibrate theoretical models predicting the temporal trend of radionuclide concentration in similar ecosystems. Moreover, information on cesium and strontium migration processes can be extended to other pollutants having similar environmental behavior.     

Preparation of [<Superscript>66</Superscript>Ga]bleomycin complex as a possible PET radiopharmaceutical

Summary Gallium-66 (T_1/2 = 9.49 h) is an interesting radionuclide that has potential use for positron emission tomography (PET) imaging of biological processes in intermediate to slow target tissue uptake. ⁶⁶Ga was produced in the NRCAM cyclotron as a result of 15 MeV proton bombardment of ⁶⁶Zn with current intensity of 180 μA (yield 11.2 mCi/μAh). Bleomycin (BLM) was labeled with [⁶⁶Ga]GaCl₃