Developing the 134Ce and 134La pair as companion positron emission tomography diagnostic isotopes for 225Ac and 227Th radiotherapeutics.

Developing targeted α-therapies has the potential to transform how diseases are treated. In these interventions, targeting vectors are labelled with α-emitting radioisotopes that deliver destructive radiation discretely to diseased cells while simultaneously sparing the surrounding healthy tissue. Widespread implementation requires advances in non-invasive imaging technologies that rapidly assay therapeutics. Towards this end, positron emission tomography (PET) imaging has emerged as one of the most informative diagnostic techniques. Unfortunately, many promising α-emitting isotopes such as 225Ac and 227Th are incompatible with PET imaging. Here we overcame this obstacle by developing large-scale (Ci-scale) production and purification methods for 134Ce. Subsequent radiolabelling and in vivo PET imaging experiments in a small animal model demonstrated that 134Ce (and its 134La daughter) could be used as a PET imaging candidate for 225AcIII (with reduced 134CeIII) or 227ThIV (with oxidized 134CeIV). Evaluating these data alongside X-ray absorption spectroscopy results demonstrated how success relied on rigorously controlling the CeIII/CeIV redox couple.

Simulation study of light transport in laser-processed LYSO:Ce detectors with single-side readout.

A tightly focused pulsed laser beam can locally modify the crystal structure inside the bulk of a scintillator. The result is incorporation of so-called optical barriers with a refractive index different from that of the crystal bulk, that can be used to redirect the scintillation light and control the light spread in the detector. We here systematically study the scintillation light transport in detectors fabricated using the laser induced optical barrier technique, and objectively compare their potential performance characteristics with those of the two mainstream detector types: monolithic and mechanically pixelated arrays. Among countless optical barrier patterns, we explore barriers arranged in a pixel-like pattern extending all-the-way or half-way through a 20 mm thick LYSO:Ce crystal. We analyze the performance of the detectors coupled to MPPC arrays, in terms of light response functions, flood maps, line profiles, and light collection efficiency. Our results show that laser-processed detectors with both barrier patterns constitute a new detector category with a behavior between that of the two standard detector types. Results show that when the barrier-crystal interface is smooth, no DOI information can be obtained regardless of barrier refractive index (RI). However, with a rough barrier-crystal interface we can extract multiple levels of DOI. Lower barrier RI results in larger light confinement, leading to better transverse resolution. Furthermore we see that the laser-processed crystals have the potential to increase the light collection efficiency, which could lead to improved energy resolution and potentially better timing resolution due to higher signals. For a laser-processed detector with smooth barrier-crystal interfaces the light collection efficiency is simulated to >42%, and for rough interfaces >73%. The corresponding numbers for a monolithic crystal is 39% with polished surfaces, and 71% with rough surfaces, and for a mechanically pixelated array 35% with polished pixel surfaces and 59% with rough surfaces.

Distribution and bioavailability of ceria nanoparticles in an aquatic ecosystem model.

Along with the increasing utilization of engineered nanoparticles, there is a growing concern for the potential environmental and health effects of exposure to these newly designed materials. Understanding the behavior of nanoparticles in the environment is a basic need. The present study aims to investigate the distribution and fate of ceria nanoparticles in an aquatic system model which consists of sediments, water, hornworts, fish and snails, using a radiotracer technique. Concentrations of ceria in the samples at regular time intervals were measured. Ceria nanoparticles were readily removed from the water column and partitioned between different organisms. Both snail and fish have fast absorption and clearance abilities. Hornwort has the highest bioaccumulation factors. At the end of the experiment, sediments accumulated most of the nanoparticles with a recovery of 75.7 ± 27.3% of total ceria nanoparticles, suggesting that sediments are major sinks of ceria nanoparticles.

Cyclotron production of radioactive CeO(2) nanoparticles and their application for in vitro uptake studies.

Nowadays, a wide variety of nanoparticles (NPs) are applied in different fields such as medical science and industry. Due to their large commercial volume, the OECD Working Party on Manufactured Nanomaterials (NMs) has proposed to study a set of 14 nanomaterials, one of which being cerium oxide (CeO(2)). In particular, CeO(2) based NPs are widely used in automotive industry, healthcare, and cosmetics. In this paper, we propose a method for the production of radioactive CeO(2) NPs.We demonstrate that they maintain the same physicochemical characteristics as the "cold" ones in terms of size distribution and Zeta potential; we develop a new protocol to assess their cellular interaction in immortalized mouse fibroblast cell line Balb/3T3, a model for the study of basal cytotoxicity and carcinogenic potential induced by chemicals and in the present case by NPs. Experimental result of this work, which shows a quasi-linear concentration-uptake response of cells, can be useful as a reference dose-uptake curve for explaining effects following biological uptake after exposure to CeO(2) NPs.

Gamma spectrum unfolding for a NaI monitor of radioactivity in aquatic systems: experimental evaluations of the minimal detectable activity.

This paper deals with the experimental evaluation of the minimal detectable activity achievable by unfolding the gamma spectra of a NaI monitor. An aquatic monitor initially developed by the Institut des Radio-Eléments (IRE) is used for the application. Unfolding of the spectra is performed with GRAVEL, a UMG package code, on the basis of a response matrix obtained with MCNP5.1.40. Experimental data have been measured at IRE, in a 20m(3) seawater tank, for known activities of (137)Cs mixed with other gamma emitters ((40)K, (133)Ba, (113)Sn and (139)Ce). Deconvolution allows one to reduce the MDA of (137)Cs by an order of magnitude.

Removal of cerium ions from aqueous solution by hydrous ferric oxide--a radiotracer study.

Radiotracer technique has been used to study the removal behavior of Ce (III) ions from aqueous solutions by synthesized and well characterized hydrous ferric oxide (HFO). Adsorptive concentration (10(-4)-10(-8) mol dm(-3)), pH (ca 4.0-10.0) and temperature (303-333 K) were examined for assessing optimal conditions for removal of these ions. The uptake of Ce (III) ions, which fitted well for Freundlich and D-R isotherms, increased with increase in the temperature and no significant desorption took place in the studied temperature range. The presence of some anions/cations affected the uptake of metal ion markedly. Irradiation of hydrous ferric oxide and tungsten oxide by using a 11.1×10(9) Bq (Ra-Be) neutron source having a neutron flux of 3.9×10(6) cm(-2) s(-1) with associated γ-dose rate of 1.72 Gy/h did not influence the extent of adsorption of Ce (III) significantly.

Impact on 141Ce, 144Ce, 95Zr, and 90Sr beta emitter dose coefficients of photon and electron SAFs calculated with ICRP/ICRU reference adult voxel computational phantoms.

The current dose coefficients for internal dose assessment of occupationally exposed persons and the general public were derived using the methodology of the International Commission on Radiological Protection (ICRP), which is similar to the Medical Internal Radiation Dose (MIRD)-type methodology. One component of this methodology is the mathematical representation of the human body (so-called MIRD-type phantoms) developed at the Oak Ridge National Laboratory for calculations of photon specific absorbed fractions (SAFs). Concerning the beta emissions, it is assumed in general that they irradiate only the organ where the radionuclide resides, whereas for walled organs, a fixed fraction of the emitted energy is absorbed within the wall. For the active marrow and bone surface targets, absorbed fractions were explicitly provided in ICRP Publication 30. The ICRP Publications 66 and 100 contain further detailed energy-dependent absorbed fraction data for the airways and the segments of the alimentary tract. In the present work, the voxel phantoms representing the reference male and female adults, recently developed at the Helmholtz Zentrum München-German Research Center for Environmental Health (HMGU) in collaboration with the Task Group DOCAL of ICRP Committee 2, were used for the Monte Carlo computation of photon as well as electron SAFs. These voxel phantoms, being constructed from computed tomography (CT) scans of individuals, are more realistic in shape and location of organs in the body than the mathematical phantoms; therefore, they provide photon SAFs that are more precise than those stemming from mathematical phantoms. In addition, electron SAFs for solid and walled organs as well as tissues in the alimentary tract, the respiratory tract, and the skeleton were calculated with Monte Carlo methods using these phantoms to complement the data of ICRP Publications 66 and 100 that are confined to self-irradiation. The SAFs derived for photons and electrons are then used to calculate the dose coefficients of the beta emitters 141Ce, 144Ce, 95Zr, and 90Sr. It is found that the differences of the dose coefficients due to the revised SAFs are much larger for injection and ingestion than for inhalation. The equivalent doses for colon and ingestion with the new voxel-based SAFs are significantly smaller than the values with the MIRD-type photon SAFs and simplifying assumptions for electrons. For lungs and inhalation, no significant difference was observed for the equivalent doses, whereas for injection and ingestion, an increase of the new values is observed.

Role of magnetite and humic acid in radionuclide migration in the environment.

Sorption of (137)Cs, (90)Sr, (154)Eu and (141)Ce by magnetite has been studied at varying pH (4 to 11) in the presence and absence of humic acid. The sorption studies have also been carried out at varying ionic strength (0.01 to 0.2 M NaClO(4)) and humic acid concentration (2 to 20 mg/L). Percentage sorption of (137)Cs and (90)Sr was found to be pH dependent, with the sorption increasing with increasing pH of the suspension. At any pH, the percentage sorption of (90)Sr was higher than that of (137)Cs. The results have been explained in terms of the electrostatic interaction between the positively charged metal ions and the surface charge of the magnetite which becomes increasingly negative with increasing pH. On the other hand, (154)Eu and (141)Ce were found to be strongly sorbed by the magnetite at all pH values, with the sorption being independent of pH. The strong sorption of trivalent and tetravalent metal ions suggests the role of complexation reactions during sorption, apart from the electrostatic interactions. However, in the case of (141)Ce surface precipitation of Ce(III) formed by reduction of Ce(IV) in the presence of magnetite cannot be ruled out. Presence of humic acid (2 mg/L) was found to have negligible effect on sorption of all metal ions.

Study on the kinetics of cerium(III) adsorption-desorption on different soils of China.

The kinetics of Ce(III) adsorption-desorption on four typical soils in China has been studied by using the batch method with the radioactive nuclide 141Ce. Results indicated that Ce(III) adsorption was rapid and nearly finished in less than 0.5 min. Desorption procedure was about completed in 1-30 min in the tested soils. Ce(III) desorption equilibrium times vary with different soils. The amounts of Ce(III) desorption on different soils in the same time were different. The Elovich equation proved to be the best models for fitting the data of Ce(III) desorption reactions in fluvo-aquic soil and black soil; and the parabolic-diffusion equation was the best model in red earth and loess soil.