Proof-of-concept studies of novel protocols for producing highly pure 48V from a 48Cr/48V generator.

The quest to improve the quality of nuclear data, such as half-lives, transition yields, and reaction cross-sections, is a shared endeavor among various areas of nuclear science. 48V is a vanadium isotope for which experimental data on neutron reaction cross-sections is needed. However, traditional isotope production techniques cannot produce 48V with high enough isotopic purity for some of these measurements. "Isotope harvesting" at the Facility for Rare Isotope Beams (FRIB) is a new isotope production technique that could potentially yield 48V with the necessary purity for such studies. In this case, 48Cr would be collected and allowed to generate 48V that can be separated from undecayed 48Cr to yield highly pure 48V. Thus, any protocol for producing pure 48V via isotope harvesting would involve utilizing a separation technique that can effectively separate 48Cr and 48V. In this study, the radiotracers 51Cr and 48V were used to develop possible radiochemical separation methodologies, which can be translated to obtain high purity 48V via this novel isotope production method. The developed protocols utilize either ion exchange or extraction chromatographic resins. Separations of 51Cr and 48V with AG 1-X8 anion exchange resin respectively resulted in recoveries of 95.6(26)% and 96.2(12)% with radionuclidic purities of 92(2)% and 99(1)%. An even more effective Cr and V separation was obtained with an extraction chromatographic resin (TRU resin) and 10 M HNO3 loading solution. Here, 51Cr and 48V respectively had recoveries of 94.1(28)% and 96.2(13)% with high radionuclidic purities (100(2)% and 100(1)%) in small volumes (8.81(8) mL and 5.39(16) mL). This study suggests that, to maximize the yield and isotopic purity of 48V, the best production protocol would involve utilizing two separations with TRU resin and 10 M HNO3 to isolate 48Cr and purify the generated 48V.

Harvesting 88Zr from heavy-ion beam irradiated tungsten at the National Superconducting Cyclotron Laboratory.

Tungsten is a commonly used material at many heavy-ion beam facilities, and it often becomes activated due to interactions with a beam. Many of the activation products are useful in basic and applied sciences if they can be recovered efficiently. In order to develop the radiochemistry for harvesting group (IV) elements from irradiated tungsten, a heavy-ion beam containing 88Zr was embedded into a stack of tungsten foils at the National Superconducting Cyclotron Laboratory and a separation methodology was devised to recover the 88Zr. The foils were dissolved in 30% hydrogen peroxide, and the 88Zr was chemically purified from the tungsten matrix and from other co-implanted radionuclides (such as 85Sr and 88Y) using strong cation-exchange (AG MP-50) chromatographic resin in sulfuric acid media. The procedure provided 88Zr in approximately 60 mL 0.5 M sulfuric acid with no detectable radio-impurities. The overall recovery yield for 88Zr was (92.3 ± 1.2)%. This proof-of-concept experiment has facilitated the development of methodologies to harvest from tungsten and tungsten-alloy parts that are regularly irradiated at heavy-ion beam facilities.

Solid-phase isotope harvesting of 88Zr from a radioactive ion beam facility.

During routine operation of the Facility for Rare Isotope Beams (FRIB), radionuclides will accumulate in both the aqueous beam dump and along the beamline in the process of beam purification. These byproduct radionuclides, many of which are far from stability, can be collected and purified for use in other scientific applications in a process called isotope harvesting. In this work, the viability of 88Zr harvesting from solid components was investigated at the National Superconducting Cyclotron Laboratory. A secondary 88Zr beam was stopped in a series of collectors comprised of Al, Cu, W, and Au foils. This work details irradiation of the collector foils and the subsequent radiochemical processing to isolate the deposited 88Zr (and its daughter 88Y) from them. Total average recovery from the Al, Cu, and Au collector foils was (91.3 ± 8.9) % for 88Zr and (95.0 ± 5.8) % for 88Y, respectively, which is over three times higher recovery than in a previous aqueous-phase harvesting experiment. The utility of solid-phase isotope harvesting to access elements such as Zr that readily hydrolyze in near-neutral pH aqueous conditions has been demonstrated for application to harvesting from solid components at FRIB.

Chitosan-TiO2 composite: A potential 68Ge/68Ga generator column material.

A durable and ready to use 68Ge-68Ga generator column material is required for its routine use in radiopharmaceutical procedures. The present work comprises preliminary studies for development and evaluation of chitosan-TiO2 based microsphere (C-TOM) composite towards its competence as a column material. The batch uptake studies showed higher distribution coefficients for 68Ge vis-à-vis 68Ga in the complete concentration range of HCl examined (0.01-1 mol.L-1). Furthermore, C-TOM showed enduring physical and chemical stability in 0.01 mol.L-1 HCl with persistent 68Ga elution profiles (>95%) and negligible 68Ge breakthrough (2 × 10-4%) for the preliminary evaluation period of ∼2 months. Overall, the studies indicated that, 68Ga with high radionuclidic purity (≥99.99%) can be eluted routinely in a small volume (∼1.5 mL) of 0.01 mol.L-1 HCl proving its potentials as a novel solid phase extractant for 68Ge/68Ge generator system.

Red Blood Cell Membrane Bioengineered Zr-89 Labelled Hollow Mesoporous Silica Nanosphere for Overcoming Phagocytosis.

Biomimetic nanoparticles (NPs) have been actively studied for their biological compatibility due to its distinguished abilities viz. long-term circulation, low toxicity, ease for surface modification, and its ability to avoid phagocytosis of NPs by macrophages. Coating the NPs with a variety of cell membranes bearing the immune control proteins increases drug efficacy while complementing the intrinsic advantages of the NPs. In this study, efforts were made to introduce oxophilic radiometal 89Zr with hollow mesoporous silica nanospheres (HMSNs) having abundant silanol groups and were bioengineered with red blood cell membrane (Rm) having cluster of differentiation 47 (CD47) protein to evaluate its long-term in vivo behavior. We were successful in demonstrating the increased in vivo stability of synthesized Rm-camouflaged, 89Zr-labelled HMSNs with the markedly reduced 89Zr release. Rm camouflaged 89Zr-HMSNs effectively accumulated in the tumor by avoiding phagocytosis of macrophages. In addition, re-injecting the Rm isolated using the blood of the same animal helped to overcome the immune barrier. This novel strategy can be applied extensively to identify the long-term in vivo behavior of nano-drugs while enhancing their biocompatibility.

Acid resistant zirconium phosphate for the long term application of 68Ge/68Ga generator system.

The 68Ge/68Ga generator system is an excellent source for producing ready-to-use Ga-68 in clinical Positron Emission Tomography (PET) applications. The column adsorbent is the key component for the 68Ge/68Ga generator system. Therefore, several studies have been conducted to identify column materials with a stable and superior elution yield in an acidic eluent (0.1 N HCl solution). In this study, four different zirconium phosphates were synthesized with a particle size of 200-800nm, pore-size of 55∼190Šand surface area of 0.72-268m2g-1. Synthesized and studied amorphous zirconium phosphate (ZrP-1) exhibited excellent acid resistant properties for the 0.1 N HCl eluent and a large surface area of 268m2g-1. Amorphous ZrP-1 showed a good Ga-68 elution yield of 74% in 0.1 N HCl eluent accompanying extraordinary low breakthrough of Ge-68 (0.007%).

Development of optical monitor of alpha radiations based on CR-39.

Fukushima accident has highlighted the need to intensify efforts to develop sensitive detectors to monitor the release of alpha emitting radionuclides in the environment caused by the meltdown of the discharged spent fuel. Conventionally, proportional counting, scintillation counting and alpha spectrometry are employed to assay the alpha emitting radionuclides but these techniques are difficult to be configured for online operations. Solid State Nuclear Track Detectors (SSNTDs) offer an alternative off line sensitive technique to measure alpha emitters as well as fissile radionuclides at ultra-trace level in the environment. Recently, our group has reported the first ever attempt to use reflectance based fiber optic sensor (FOS) to quantify the alpha radiations emitted from (232)Th. In the present work, an effort has been made to develop an online FOS to monitor alpha radiations emitted from (241)Am source employing CR-39 as detector. Here, we report the optical response of CR-39 (on exposure to alpha radiations) employing techniques such as Atomic Force Microscopy (AFM) and Reflectance Spectroscopy. In the present work GEANT4 simulation of transport of alpha particles in the detector has also been carried out. Simulation includes validation test wherein the projected ranges of alpha particles in the air, polystyrene and CR-39 were calculated and were found to agree with the literature values. An attempt has been further made to compute the fluence as a function of the incidence angle and incidence energy of alphas. There was an excellent correlation in experimentally observed track density with the simulated fluence. The present work offers a novel approach to design an online CR-39 based fiber optic sensor (CRFOS) to measure the release of nanogram quantity of (241)Am in the environment.

Determination of alpha activity in organic solvents using CR-39.

Solid State Nuclear Track Detector (SSNTD) like CR-39 offers a unique opportunity to measure alpha radiations in a complex matrix like high level nuclear waste due to its sensitivity to only alpha radiations in the presence of intense beta-gamma radiation field. There is however a concern about the lower sensitivity of SSNTD when the radiation source is present in solution vis-à-vis solid medium. The sensitivity of CR-39 toward detection of alpha particles homogenously distributed in n-hexane, n-dodecane and n-octanol has been investigated and was found to be better than that obtained in 3 M HNO3.

A novel approach for preferential recovery of Sr from (Sr, Th)O2.

Quantitative leaching of Sr from homogeneous and calcined (Th,Sr) O(2) in dilute perchloric acid medium suggests the possibility of reducing the hazardousness of discharged nuclear fuel by separation of (90)Sr, a prominent fission product at dissolution stage itself rather than the conventional approach of its recovery from high level nuclear waste. Apart from mitigating the radiotoxicity of the nuclear waste, recovered (90)Sr can be employed as a compact heat source and as parent radionuclide for (90)Y (used in therapy radiopharmaceuticals), provided it can be made available at desired high purity. Leaching behavior of few other fission products was also investigated to quantify their contamination in leached Sr. Feasibility of employing extraction chromatography using Sr selective resin was explored in perchloric acid medium. In this context, the distribution coefficients of (85)Sr(II), Th (IV), Zr(IV), Y(III), Pd(II) as well as (152)Eu(III) and (137)Cs (I) were determined under varying nitric acid/perchloric acid concentration and under varying loading conditions of metal ions. Perchloric acid medium appears better than nitric acid medium for preferential leaching of Sr from (Th,Sr)O(2) as well as for uptake of Sr by Sr selective chromatographic resin.