Reactor production of anhydrous18F ion

The direct production of anhydrous¹³F ion has been achieved through the incorporation of a new approach to hot atom reactions for reactor generated radiopharmaceuticals. Capitalizing on the traditional Li₂CO₃ method for hydrated¹⁸F production, a unique target design and geometry utilizing neutron generated energetic tritions emerging from the surface of a thin LiF embedded stainless steel matrix react with gaseous O₂ to produce¹⁸F as a free recoiling anhydrous species. Approximately 10–15 MBq of reactive anhydrous¹⁸F ion absorbed onto a metallic foil has been produced by this method. Verification of the production of¹⁸F was substantiated through decay measurements using Ge(Li) spectroscopic analysis, and by the synthesis of¹⁸F-fluoromethane gas. Cyclotron gas target chemistry which has been instrumental in the preparation of¹⁸F-2FDG and other metabolic tracers may be reproduced using this technique by the addition of 1% F₂ scavenger gas to a recirculating reactor gas handling system.     

A feasibility study of the cyclotron production of21Na

The cyclotron production of²¹Na, via the²⁰Ne(d, n)²¹Na and the²⁰Ne(³He, pn)²¹Na and²⁰Ne(³He, 2n)²¹Mg ²¹Na nuclear reactions, has been investigated. Transfer of²¹Na from the production target to the medical application site some 10 m distant was achieved by gas phase and liquid phase systems, both of which are described. Under optimal conditions 111 MBq·ml^–1 (3 mCi·ml^–1) of²¹Na were available at the dispensing reservoir 10 m distant from the production target, when irradiating with a 5 A deuteron beam current. Incident deuteron energy was degraded to below 3.0 MeV by a 350 m Al entrance foil, to avoid production of¹⁸F. The charge distribution of²¹Na inside the production target and inside the gas phase transfer tube at distances of 1 m and 15 m were determined, and are reported along with data from similar studies during¹⁸F production via the²⁰Ne(d, )¹⁸F reaction.²¹Na accumulated primarily at the cathode, indicating the production of positively charged species, whereas¹⁸F was equally distributed between the electrodes in a production target constructed especially for measuring the charge distribution of the radioactive species.     

Determination of oxygen impurity in high purity materials by charged particle activation analysis using alpha projectiles

40 MeV -particles have been used to determine oxygen impurity at ppm levels in silicon, copper, and stainless steel, through the radiochemical separation of¹⁸F from the matrix. The separation of¹⁸F has been carried out by two techniques, viz.(1) distillation of H₂SiF₆ and (2) precipitation of KBF₄ and some modification has been applied in the separation, depending on the nature of interferences from the matrix. Instrumental approach was also carried out to determine the oxygen impurity at 100 ppm in Si matrix because this approach is not possible in Cu and stainless steel samples due to matrix activity.     

Production of123I using the CV-28 cyclotron at IPEN-CNEN/SP

These studies had the purpose of establishing the optimal conditions for the production of¹²³I through the¹²⁴Te (p, 2n)¹²³I reaction, using the CV-28 Cyclotron (E_max=24 MeV for protons) at IPEN-CNEN/SP. Two different targets (TeO₂ and TeO₂+2% Al₂O₃) were irradiated in order to check their physical resistance against beam current (up to 12 A) and length of irradiation (10 min — 2h), and to evaluate the recovery of the radioiodine produced, by a dry distillation process with a high frequency induction furnace. Later on, enriched¹²⁴TeO₂ (96.2%) targets were irradiated, and¹²³I was produced routinely with a production yield of (3. 31±0.07) mCi/Ah, 1.7% of¹²⁴I at EOB and radiochemically pure.     

Remotely controlled on-line production of different species labeled with15O

For on-line production of [¹⁵O]–O₂, [¹⁵O]–CO₂, [¹⁵O]–CO, and [¹⁵O]–H₂O, a new apparatus was assembled. The yield at a beam current of 10 A and a flow rate of 750 ml min^–1 was about 110 MBq ml^–1 target gas or 93 MBq ml^–1 H₂O at steady state.     

Alpha-activation analysis of nitrogen in boron-doped silicon single crystal

The rapid dissolution of silicon and the substoichiometric separation of¹⁸F were studied in order to determine nitrogen in a boron-doped silicon single crystal by activation analysis via¹⁵N(,n)¹⁸F. The silicon dissolution method was developed by using a nitric acid-based solution containing a known amount of ammonium fluoride, instead of hydrofluoric acid, as the¹⁸F carrier. The silicon could be dissolved to a depth of 100 m with a 10 mm Ø in 9 minutes. The conditions for¹⁸F steam distillation and substoichiometric precipitation as lanthanum fluoride were improved. 50% of the fluorine could be separated substoichiometrically even though the carrier amount was increased from 6–12 mmol to more than 16 mmol in order to add it to the dissolving solution. This dissolution method and improved substoichiometric separation were used to determine nitrogen in a boron-doped silicon single crystal. The nitrogen concentration was found to be less than the detection limit (50 ppb).     

Efficiency of an in-line charcoal filter in automated chemistry process control unit during the synthesis of18F-fluorodeoxyglucose (FDG)

¹⁸F fluoride ion is produced by bombarding¹⁸O enriched water using an 11 MeV negative ion Radioisotope Delivery System (RDS-112) cyclotron by¹⁸O(p,n)¹⁸F reaction. During the synthesis of¹⁸F-FDG, a gaseous effluent containing¹⁸F is released. To quantitate the loss of¹⁸F during the synthesis, the¹⁸F activity at the end of bombardment delivered to chemical process control unit (CPCU), the amount of¹⁸F-FDG produced, the residual activity in CPCU, the activity trapped in charcoal filter, reaction vessels, cartridge and resin column were measured. A dose calibrator was used to assay total¹⁸F delivered to the CPCU and FDG produced. All other measurements were with a calibrated ionization chamber in a fixed geometry. The amount of gaseous¹⁸F released was calculated. For routine productions, conversion of¹⁸F into FDG was 46.0±4.0%. In six production runs without a charcoal filter, the mean gaseous release of¹⁸F was 10.6±1.0%. With an activated charcoal filter retrofitted to the exhaust of the CPCU, then mean gaseous¹⁸F activity released was 1.2±1.2%. The residual activity in the synthesis unit was 12.9±3.5%. The remaining activity i.e. 33.1±4.2%, was in the reaction vessels, cartridges and in the resin column. The efficiency of a charcoal filter for trapping¹⁸F gaseous effluent during synthesis was found to be >99.0%.     

Determination of fluorine in standard rocks by photon activation analysis

A highly sensitive determination of fluorine in standard rocks by photon activation using the¹⁹F(,n)¹⁸F reaction combined with pyrohydrolysis for the separation of¹⁸F has been reported. The irradiation energy was operated at 20 MeV to avoid the interference from Na, because Na is one of the major element in rocks and¹⁸F is also produced from Na via²³Na(,n)¹⁸F reaction above its threshold energy, 20.9 MeV. After irradiation, fluorine was extracted by pyrohydrolysis and separated as LaF₃ precipitate. It was ascertained that the average recovery of fluorine in standard rocks was about 90% and the precipitate was of high radiochemical purity. This method was applied to the analysis of ten GSJ rock reference samples and two USGS standard rocks issued by the Geological Survey of Japan and the United States Geological Survey, respectively. The detection limit of this method was 0.02 g/g, and the results obtained by this method were in good agreement with the recommended values. This method was easily applied to the determination of a few ppm level of fluorine in rock samples, such as ultrabasic rock and feldspar.     

Reactions parasites rencontrees lors du dosage de l’oxygene dans le silicium au moyen des particules alpha

Activation analysis by charged particles may encounter great difficulties when ‘parasitic’ reactions induce in the matrix itself the same radionuclide as the one requested by the reaction for analytical aim. In this investigation we study reactions inducing¹⁸F activity in silicon and we show the importance of these reactions for determining low levels of oxygen in silicon by the reactions \(O\mathop \to \limits^\alpha {}^{18}F\) . For irradiations carried out with 54 MeV α-particles, the profile of¹⁸F production in silicon presents an activity decreasing very rapidly from the surface to depths of 500 μm without any connection with the \(O\mathop \to \limits^\alpha {}^{18}F\) activation curve. The diffusion of¹⁸F nuclides created at the surface from the oxide bed does not at all explain that result. The differences between these curves are attributed to parasitic reactions inducing¹⁸F activity in silicon. In order to confirm the reaction \(Si\mathop \to \limits^\alpha {}^{18}F\) we also investigated the profile of²⁴Na and²⁹Al production by another parasitic reaction in silicon. It is pointed out that the choice of incident energy is quite primordial, for analyses of oxygen in silicon with 54 MeV α-particles are not quite suitable. The best energy range appears to be around 35 MeV.     

Production of 6-l-[18F]Fluoro-m-tyrosine in an Automated Synthesis Module for 11C-Labeling

6-l-[¹⁸F]Fluoro-m-tyrosine (6-l-[¹⁸F]FMT) represents a valuable alternative to 6-l-[¹⁸F]FDOPA which is conventionally used for the diagnosis and staging of Parkinson’s disease. However, clinical applications of 6-l-[¹⁸F]FMT have been limited by the paucity of practical production methods for its automated production. Herein we describe the practical preparation of 6-l-[¹⁸F]FMT using alcohol-enhanced Cu-mediated radiofluorination of Bpin-substituted chiral Ni(II) complex in the presence of non-basic Bu₄ONTf using a volatile iPrOH/MeCN mixture as reaction solvent. A simple and fast radiolabeling procedure afforded the tracer in 20.0 ± 3.0% activity yield within 70 min. The developed method was directly implemented onto a modified TracerLab FX C Pro platform originally designed for ¹¹C-labeling. This method enables an uncomplicated switch between ¹¹C- and ¹⁸F-labeling. The simplicity of the developed procedure enables its easy adaptation to other commercially available remote-controlled synthesis units and paves the way for a widespread application of 6-l-[¹⁸F]FMT in the clinic.     

Aspects of the chemistry of SF6/O2 plasmas

The production ofSOF ₄ initiated by the reaction of F atoms withSOF ₂ has been studied in a gas-flow reactor at 295 K for helium bath gas number densities in the range (3.0–27.0)×10¹⁶ cm^–3. The effect of O atoms on the formation ofSOF ₄ has been analyzed in terms of the competing reactionsSOF ₃+FSOF₄ andSOF ₃+OSO ₂ F ₂+F. This analysis leads to the conclusion that the rate coefficients for these two processes are equal within an uncertainty of about 50%. Furthermore, both experiment and calculations indicate that the rate coefficient for reactions between F atoms andSOF ₃ is close to its high-pressure limit under the conditions employed. The experiments set a lower limit on this rate coefficient of 5×10^–11 cm³ s^–1, while calculations based on unimolecular rate theory suggest that it may be greater than 1×10^–10 cm³ s^–1. These results make it clear that the two reactions shown above cannot explain the relative abundances ofSOF ₄ andSO ₂ F ₂ which are observed inSF ₆/O ₂ plasmas. This suggests thatSF ₂ is a major precursor in the sequence of reactions following the dissociation ofSF ₆.     

In situ 18F-γ-ray-induced Ag nanoparticle formation in the presence of SiO2 nanoparticles under air

The in situ ¹⁸F-γ-ray irradiation of SiO₂ nanoparticles in an aqueous solution containing Ag⁺ led to the reduction of Ag⁺ to Ag⁰ aggregates or Ag⁰ nanoparticles in a small volume (0.1 ml) under air. ¹⁸F was used in the form of ¹⁸F-fluorodeoxyglucose, produced by a cyclotron at our University hospital. The in situ average absorbed dose at the distance of 1 µm in the solution volume (0.1 ml) was calculated to be 12.2 kGy equivalent to a point source of 20 MBq. The SiO₂ nanoparticles had two effects; they enhanced the reduction of Ag⁺ to Ag⁰ aggregates and they acted as reaction sites to prevent aggregation. When Ag⁺ adsorbed on the surface of the SiO₂ nanoparticles, Ag nanoparticles were formed by ¹⁸F γ-rays. The absorption spectra of Ag nanoparticles and Ag⁰ aggregates were markedly different.     

Oxygen isotope measurement by instrumental neutron activation analysis using reactor neutron—Revisited

The oxygen isotopes¹⁶O and¹⁸O were determined using reactor instrumental neutron activation analysis by utilizing the¹⁶O(n, p)¹⁶N and the¹⁸O(n, )¹⁹O reaction in the UCI 250 kw TRIGA research reactor.¹ Such measurements were used to follow an exchange reaction between H₂ ¹⁸O and finely ground coal. The best conditions for the determination were explored and interference reactions quantified. Single irradiation/count sequences were used to determine 30 parts per thounsand of¹⁶O and 1 part per thousand of¹⁸O in a 400 mg sample of an HVA rank coal to a 25% (1) precision. Reactor pulses were shown to improve these detection limits significantly. Special attention was given to correcting for the high count rates from other induced activites.     

Effect of the specific activity of the tracer on rat luteinizing hormone radioimmunoassay

Rat luteinizing hormone /LH/ was labelled with¹²⁵I by the Chloramine T method.¹²⁵I-LH, used as tracer in radioimmunoassay, was separated from the labelling reaction mixture by gel filtration. By using the proper protein/radioiodine ratio in the labelling reaction mixture the specific activity of¹²⁵I-LH was adjusted to 2.5–20.5 MBq g^–1. The influence of the specific activity on the assay parameters as well as on the tracer stability was investigated.     

Osmotic Coefficients of Aqueous Solutions of Some Poly(oxyethylene) Glycols at the Freezing Point of Solution

The freezing temperatures of dilute aqueous solutions of some poly(oxyethylene) glycols (PEG, HO–(CH₂CH₂O) _n –H, n varying from 4 to 117) were measured over a solute to solvent mass ratio from 0.0100 to 0.3900. The second and third osmotic virial coefficient (A ₂₂ and A ₂₂₂) of poly(oxyethylene) glycols in aqueous solution were determined. The molecular weight dependence of the second virial coefficient can be described by a simple relation A ₂₂=2×10^–5 M _n ^1.86, and the third virial coefficient is A ₂₂₂=0.038A ₂₂ ². The activity coefficients of the solute were calculated using the Gibbs-Duhem equation as applied by Bjerrum. From the osmotic and activity coefficients the excess Gibbs energies of solution, as well as the respective partial molar functions of solute and solvent and the virial pair interaction coefficients for the excess Gibbs energies were estimated. The second and the third osmotic virial coefficients are correlated with the Mc-Millan-Mayer virial coefficients.     

The biological half-life of137Cs in snails

The biological half-life of¹³⁷Cs in snails Helix pomatia after a single administration of contaminated diet has been investigated. The calculation was based on the retention of¹³⁷Cs in snails in vivo. It was found that loss of cesium from snails can be explained by a two-exponential retention curve leading to biological loss constants _{B 1}=0.27 d^–1 and _{B 2}=0.024 d^–1, which correspond to biological half-lives of T_{B 1}=2.5 d and T_{B 2}=28.5 d respectively. The equation describing the retention of¹³⁷Cs in snails is also presented.     

Estimated ionicB-coefficients from NMR measurements in aqueous electrolyte solutions

¹⁷O-NMR spin-lattice relaxation timesT ₁ of D₂O molecules were measured at 5–85°C in D₂O solutions of alkali metal halides (LiClCsCl, KBr, and KI), DCl, KOD, Ph₄PCl, NaPh₄B, and tetraalkylammonium bromides (Me₄NBrAm₄NBr) in the concentration range 0.1–1.4 mol-kg^–1 TheB-coefficients of the electrolytes obtained from the concentration dependence of relaxation ratesR ₁=1/T₁ were divided into the ionicB-coefficients by three methods: (i) the assumption ofB (K⁺)=B(Cl^–), (ii) the assumption ofB(Ph₄P⁺)=B(Ph₄B^–), and (iii) the use ofB(Br^–) obtained from a series ofB(R₄NBr). It was found that Methods (ii) and (iii) resulted in an abnormal temperature dependence of theB-coefficients of alkali metal ions and a negative values of rotational correlation times _c at lower temperatures for hydroxide and halide ions. These results suggest that the methods based on the van der Waals volume are not adequate for the ionic separation of NMRB-coefficients. From the analysis using the assumption ofB(K⁺)=B(Cl^–), it was found that D₃O⁺, OD^–, and Me₄N⁺ ions are the intermediates between structure makers and breakers, and that the hydrophobicity of phenyl groups is weaker than that of alkyl groups due to the interactions between water molecules and -electrons in phenyl groups.     

Synthesis of [F]xenon difluoride as a radiolabeling reagent from [F]fluoride ion in a micro-reactor and at production scale

[¹⁸F]Xenon difluoride ([¹⁸F]XeF₂), was produced by treating xenon difluoride with cyclotron-produced [¹⁸F]fluoride ion to provide a potentially useful agent for labeling novel radiotracers with fluorine-18 (t_1/2 = 109.7 min) for imaging applications with positron emission tomography. Firstly, the effects of various reaction parameters, for example, vessel material, solvent, cation and base on this process were studied at room temperature. Glass vials facilitated the reaction more readily than polypropylene vials. The reaction was less efficient in acetonitrile than in dichloromethane. Cs⁺ or K⁺ with or without the cryptand, K 2.2.2, was acceptable as counter cation. The production of [¹⁸F]XeF₂ was retarded by K₂CO₃, suggesting that generation of hydrogen fluoride in the reaction milieu promoted the incorporation of fluorine-18 into xenon difluoride. Secondly, the effect of temperature was studied using a microfluidic platform in which [¹⁸F]XeF₂ was produced in acetonitrile at elevated temperature (≥85 °C) over 94 s. These results enabled us to develop a method for obtaining [¹⁸F]XeF₂ on a production scale (up to 25 mCi) through reaction of [¹⁸F]fluoride ion with xenon difluoride in acetonitrile at 90 °C for 10 min. [¹⁸F]XeF₂ was separated from the reaction mixture by distillation at 110 °C. Furthermore, [¹⁸F]XeF₂ was shown to be reactive towards substrates, such as 1-((trimethylsilyl)oxy)cyclohexene and fluorene.     

Fragmentation of the valence electronic states of NF3 studied by threshold photoelectron–photoion coincidence spectroscopy

The valence threshold photoelectron spectrum of NF₃ is reported for the first time in the literature, and threshold photoelectron–photoion coincidence (TPEPICO) spectroscopy has measured, state-selectively, the decay dynamics of the valence states of NF₃⁺ in the range 13–23 eV. Vacuum–UV radiation from the Daresbury synchrotron source dispersed by a 1 m Seya-Namioka monochromator photoionises the parent molecules. Electrons and ions are detected by threshold electron analysis and time-of-flight mass spectrometry, respectively. TPEPICO spectra are recorded continuously as a function of photon energy, allowing coincidence ion yields of the fragment ions and the breakdown diagram to be obtained. A comparison of the integrated threshold photoelectron and the total ion signals as a function of energy suggests that, in the range 16–19 eV, autoionisation via Rydberg states of NF₃ makes a significant contribution to the production of threshold electrons. The 50% crossover energy for production of NF₂⁺ from NF₃⁺ is determined to be 14.10±0.05 eV. The first onsets for NF₂⁺ and NF⁺ production are 13.95±0.05 and 17.6±0.1 eV, respectively. The majority of the Franck–Condon region of the ground state of NF₃⁺ is stable with respect to dissociation to NF₂⁺, whereas the unresolved states and most of the state dissociate exclusively to NF₂⁺. The and states dissociate to NF⁺. Translational kinetic energy releases have been measured in NF₂⁺ and NF⁺ at the energies of the Franck–Condon maxima of the valence states of NF₃⁺. The results are compared with models assuming statistical and impulsive dissociation. The Ã/ states of NF₃⁺ dissociate directly from the excited-state potential energy surface to NF₂⁺, whereas the higher-lying state probably dissociates off the ground-state surface following rapid internal conversion. It is not possible to correlate unambiguously the formation of NF⁺ with either F₂ or 2F, although on energetic grounds the latter products are more likely. Assuming that the neutral products are 2F, no information is obtained whether the two N–F bonds break simultaneously or sequentially.     

Isotope effect of retention value between64Cu and66Cu in neutron-irradiated copper phthalocyanine

Copper phthalocyanine ( and forms) in neat solid or in dissolved state in conc. H₂SO₄ was neutron-irradiated, and retention values of⁶⁴Cu and⁶⁶Cu were estimated to study whether or not there is any isotope effect in retention between these two (n, )-produced radionuclides. The data show that there is an isotope effect expressed by the ratio of retention of⁶⁶Cu to that of⁶⁴Cu, ranged from 1.29±0.12 for form dissolved in conc. H₂SO₄ to 1.09±0.02 for form in neat solid irradiation. This result coincides with the tendency anticipated from the recoil energy spectra which were computed by a program using Monte-Carlo method.