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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Optimized anion exchange column isolation of zirconium-89 (89Zr) from yttrium cyclotron target: Method development and implementation on an automated fluidic platform

Zirconium-89 (89Zr), produced by the (p,n) reaction from naturally monoisotopic yttrium (natY), is a promising positron emitting isotope for immunoPET imaging. Its long half-life of 78.4 h is sufficient for evaluating slow physiological processes. A prototype automated fluidic system, coupled to on-line and in-line detectors, has been constructed to facilitate development of new 89Zr purification methodologies. The highly reproducible reagent delivery platform and near-real time monitoring of column effluents allows for efficient method optimization. The separation of Zr from dissolved Y metal targets was evaluated using several anion exchange resins. Each resin was evaluated against its ability to quantitatively capture Zr from a load solution that is high in dissolved Y. The most appropriate anion exchange resin for this application was identified, and the separation method was optimized. The method is capable of a high Y decontamination factor (>105) and has been shown to separate Fe, an abundant contaminant in Y foils, from the 89Zr elution fraction. Finally, the performance of the method was evaluated using cyclotron bombarded Y foil targets. The separation method was shown to achieve >95% recovery of the 89Zr present in the foils. The 89Zr eluent, however, was in a chemical matrix not immediately conducive to labeling onto proteins. The main intent of this study was to develop a tandem column 89Zr purification process, wherein the anion exchange column method described here is the first separation in a dual-column purification process.

Zirconium-89, ImmunoPET, medical isotope, automati↗
DOE OSTI2022

Anion exchange and extraction chromatography tandem column isolation of zirconium-89 ( 89 Zr) from cyclotron bombarded targets using an automated fluidic platform

The long-lived positron emitter 89 Zr is a highly promising nuclide employed in diagnostic Positron Emission Tomography (PET) imaging. Methods of radiochemical processing to obtain 89 Zr for clinical use are traditionally performed with a single hydroxamate resin column. In this work, we present a tandem column purification method for the preparation of high-purity 89 Zr from cyclotron bombarded Y metal foils. The primary column is a macroporous, strongly basic anion exchange resin on styrene divinylbenzene co-polymer. The secondary microcolumn, with an internal volume of 33 µL, is packed with an extraction chromatography resin (ExCR) loaded with HDEHP. A condition of “inverted selectivity” is presented, wherein the 89 Zr elution from the primary column is synonymous with the load condition on the secondary column. The ability to transfer 89 Zr from one column to the next allows two sequential column clean-up methods to be performed prior to the final elution of the 89 Zr product. This approach assures delivery of very high purity 89 Zr . The tandem column purification process has been implemented into a prototype automated fluidic system. Optimization of the method is presented, followed by evaluation of the process using seven cyclotron bombarded Y metal foil targets. Once optimized, we found that 93.7±2.3% of the 89 Zr present in the foils was recovered in the secondary column elution fraction (0.8 M oxalic acid). Radiochromatograms of the product elution peaks enabled determination of full width at half-maximum (FWHM) and 89 Zr collection yields as a function of volume. Because of the small size of the secondary microcolumn, a 89 Zr product volume of ~0.28 mL is reported, which provides a substantially increased nuclide concentration over traditional methods. Finally, we evaluated the transchelation of the resulting 89 Zr oxalate product to deferoxamine mesylate (DFOM) salt. We observed effective specific activities (ESA) and bindable metals concentrations ([M B ]) that exceed those reported by the traditional single hydroxamate column method.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2013

Nuclear Data Sheets for A = 89

The evaluated experimental data are presented for 14 known nuclides of mass 89 (Ge, As, Se, Br, Kr, Rb, Sr, Y, Zr, Nb, Mo, Tc, Ru, Rh). New data on high–spin excitations are available for {sup 89}Kr, {sup 89}Rb, {sup 89}Sr, {sup 89}Tc and {sup 89}Ru, including a superdeformed structure in {sup 89}Tc. Fluorescence studies in {sup 89}Y have revealed a large number of new levels in 7–11 MeV range. New two–neutron transfer data are available for {sup 89}Zr. New direct and precise measurement of atomic masses of {sup 89}Se, {sup 89}Br, 89{sup K}r, {sup 89}Rb, {sup 89}Mo and {sup 89}Tc have greatly improved the Q value landscape in this mass region. This work supersedes previous A=89 evaluation published in 1998Si31, and also the older ones 1989Si20, 1975Ko21, and M.W. Johns et al., Nuclear Data Tables A 8, 373 (1970). In spite of extensive experimental work on the isobaric nuclei of this mass chain several deficiencies remain. The identification of {sup 89}Rh isotope remains unconfirmed. The half–lives of ground states of {sup 89}Ge, {sup 89}As and {sup 89}Rh have not been measured, only the lower limits are estimated from time–of–flight in a reaction and experimental arrangement, where produced and identified. The decay schemes of {sup 89}Ge, {sup 89}As, {sup 89}Se, {sup 89}Ru and {sup 89}Rh are not known, and those for {sup 89}Tc and {sup 89}Mo are incomplete. High–lying (neutron unbound) levels in {sup 89}Kr, expected to be populated in the decay of {sup 89}Br, have not been investigated. The spins and parities for levels in {sup 89}Kr are largely unassigned, while for {sup 89}Tc and {sup 89}Ru, only few low–spin excitations are established. For {sup 89}Rb, little information is available for high–spin structures. Detailed gamma–ray data are available for {sup 88}Sr(n,γ){sup 89}Sr reaction, but most of these γ rays remain unassigned in a level scheme. Excited state data are nonexistent for {sup 89}Ge, {sup 89}As, {sup 89}Se, {sup 89}Br and {sup 89}Rh. The {sup 89}Y and {sup 89}Zr are the most extensively studied nuclei in A=89.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2018

Spectral-average cross section validation in LR-0 reactor spectrum of {sup 55}Mn(n,2n), {sup 90}Zr(n,2n) and {sup 127}I(n,2n) reactions - 25362

This article deals with the validation of spectral average cross-sections (SACS) of {sup 55}Mn(n,2n){sup 54}Mn, {sup 90}Zr(n,2n){sup 89}Zr and {sup 127}I(n,2n){sup 126}I reactions in well-defined LR-0 reactor spectrum. The measurement of SACS for selected reactions is of high interest because they are used for the practical reactor dosimetry and also for refinement of prompt fission neutron spectra of {sup 235}U in the region of higher energies. Various experiments for description of neutron field in reactor and detector characterization, which are necessary for validation, are described. The spectral average cross-sections are derived from Net Peak Areas of irradiated samples measured using a semiconductor high purity germanium detector. The spectral average cross section in {sup 235}U prompt fission neutron spectrum was experimentally determined to be 0.239 ± 0.015 mb for {sup 55}Mn, 1.209 ± 0.052 mb for {sup 127}I and 0.107 ± 0.005 mb for {sup 90}Zr. The obtained results were compared with MCNP6 calculations using ENDF/B-VII.0, ENDF/B-VII.1, JEFF-3.1, JEFF-3.2, JENDL-3.3, JENDL-4, ROSFOND-2010, CENDL-3.1 and IRDFF-1.05 nuclear data libraries. Notable discrepancies were found in {sup 90}Zr(n,2n){sup 89}Zr and {sup 127}I(n,2n){sup 126}I reactions. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2018

A 89 Zr-labeled lipoplex nanosystem for image-guided gene delivery: design, evaluation of stability and in vivo behavior

Background: With the advances in radiopharmaceutical research, the development of image-guided therapy has become a major interest. While the development of theranostic nanotherapeutics is frequently associated with cancer chemotherapy, phototherapy and radiotherapy, there is little information available on the in vivo monitoring of gene delivery systems and the application of image-guided approach in gene therapy. The goal of this work was to determine the in vivo behavior of DNA delivery nanosystems - based on cationic gemini surfactants – designed for image-guided gene therapy. We tested the feasibility of monitoring tumor accumulation of gene delivery nanoparticles by positron emission tomography. Methods: To be able to conjugate radiotracers to the nanoparticles, a deferoxamine-modified gemini surfactant was synthesized, DNA-containing lipoplex nanoparticles were formulated, and radiolabeled with Zirconium-89 ( 89 Zr). The pharmacokinetics and biodistribution of 89 Zr labeled surfactant and 89 Zr labeled nanoparticles were monitored in mice by microPET/CT imaging and ex vivo gamma counting. Results: Modification of the nanoparticles with deferoxamine did not alter their physicochemical properties. The radiolabeled nanoparticles (labeling efficiency of 95±3%) were stable in PBS and serum. The biological half-life of the 89Zr labeled nanoparticles was significantly higher compared to 89Zr labeled surfactant. As expected, the nanoparticles had significantly higher liver accumulation than the radiolabeled surfactant alone and lower kidney accumulation. Tumor uptake was detected at 2 hours post injection and decreased throughout the 3-day monitoring. Conclusion: We propose that radiolabeling DNA delivery lipoplex nanosystems is a promising approach for the design and optimization of image-guided nanomedicines, especially in the context of cancer gene therapy.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2012

Enhanced NIF neutron activation diagnostics

The NIF neutron activation diagnostic suite relies on removable activation samples, leading to operational inefficiencies and a fundamental lower limit on the half-life of the activated product that can be observed. A neutron diagnostic system measuring activation of permanently installed samples could remove these limitations and significantly enhance overall neutron diagnostic capabilities. The physics and engineering aspects of two proposed systems are considered: one measuring the {sup 89}Zr/{sup 89m}Zr isomer ratio in the existing Zr activation medium and the other using potassium zirconate as the activation medium. Both proposed systems could improve the signal-to-noise ratio of the current system by at least a factor of 5 and would allow independent measurement of fusion core velocity and fuel areal density.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

p-SCN-Bn-HOPO: A Superior Bifunctional Chelator for 89 Zr ImmunoPET

Zirconium-89 has an ideal half-life for use in antibody-based PET imaging; however, when used with the chelator DFO, there is an accumulation of radioactivity in the bone, suggesting that the 89 Zr 4+ cation is being released in vivo. Therefore, a more robust chelator for 89 Zr could reduce the in vivo release and the dose to nontarget tissues. Evaluation of the ligand 3,4,3-(LI-1,2-HOPO) demonstrated efficient binding of 89 Zr 4+ and high stability; therefore, we developed a bifunctional derivative, p-SCN-Bn-HOPO, for conjugation to an antibody. A Zr-HOPO crystal structure was obtained showing that the Zr is fully coordinated by the octadentate HOPO ligand, as expected, forming a stable complex. p-SCN-Bn-HOPO was synthesized through a novel pathway. Both p-SCN-Bn-HOPO and p-SCN-Bn-DFO were conjugated to trastuzumab and radiolabeled with 89 Zr. Both complexes labeled efficiently and achieved specific activities of approximately 2 mCi/mg. PET imaging studies in nude mice with BT474 tumors (n = 4) showed good tumor uptake for both compounds, but with a marked decrease in bone uptake for the 89 Zr-HOPO-trastuzumab images. Biodistribution data confirmed the lower bone activity, measuring 17.0%ID/g in the bone at 336 h for 89 Zr-DFO-trastuzumab while 89 Zr-HOPO-trastuzumab only had 2.4%ID/g. We successfully synthesized p-SCN-Bn-HOPO, a bifunctional derivative of 3,4,3-(LI-1,2-HOPO) as a potential chelator for 89 Zr. In vivo studies demonstrate the successful use of 89 Zr-HOPO-trastuzumab to image BT474 breast cancer with low background, good tumor to organ contrast, and, importantly, very low bone uptake. The reduced bone uptake seen with 89 Zr-HOPO-trastuzumab suggests superior stability of the 89 Zr-HOPO complex.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2014

TU-F-12A-01: Quantitative Non-Linear Compartment Modeling of 89Zr- and 124I- Labeled J591 Monoclonal Antibody Kinetics Using Serial Non-Invasive Positron Emission Tomography Imaging in a Pre-Clinical Human Prostate Cancer Mouse Model

Purpose: To examine the binding kinetics of human IgG monoclonal antibody J591 which targets prostate-specific membrane antigen (PSMA) in a pre-clinical mouse cancer model using quantitative PET compartmental analysis of two radiolabeled variants. Methods: PSMA is expressed in normal human prostate, and becomes highly upregulated in prostate cancer, making it a promising therapeutic target. Two forms of J591, radiolabeled with either {sup 89}Zr or {sup 124}I, were prepared. {sup 89}Zr is a radiometal that becomes trapped in the cell upon internalization by the antigen-antibody complex, while radioiodine leaves the cell. Mice with prostate cancer xenografts underwent non-invasive serial imaging on a Focus 120 microPET up to 144 hours post-injection of J591. A non-linear compartmental model describing the binding and internalization of antibody in tumor xenograft was developed and applied to the PET-derived time-activity curves. The antibody-antigen association rate constant (ka), total amount of antigen per gram tumor (Ag-total), internalization rate of antibody-antigen complex, and efflux rate of radioisotope from tumor were fitted using the model. The surface-bound and the internalized activity were also estimated. Results: Values for ka, Ag-total, and internalization rate were found to be similar regardless of radiolabel payload used. The efflux rate, however, was ∼ 9-fold higher for {sup 124}I-J591 than for {sup 89}Zr-J591. Time-dependent surface-bound and internalized radiotracer activity were similar for both radiolabels at early times post-injection, but clearly differed beyond 24 hours. Conclusion: Binding and internalization of J591 to PSMA-expressing tumor xenografts were similar when radiolabeled with either {sup 89}Zr or {sup 124}I payload. The difference in efflux of radioactivity from tumor may be attributable to differential biological fate intracellularly of the radioisotopes. This has great significance for radioimmunotherapy and antibody-drug conjugates. Further exploration using the model will examine binding and radioisotope residence as antibody dose is increased to antigen saturation. The Center for Targeted Radioimmunotherapy and Theranostics, Ludwig Center for Cancer Immunotherapy, Memorial Sloan Kettering Cancer Center (MSK), NIH (R25-CA096945). Technical services provided by the MSK Small-Animal Imaging Core Facility were supported by the NIH (R24-CA83084, P30-CA08748, and P50-CA92629; Zanzonico). NCI, Center to Reduce Cancer Health Disparity (R21 CA153177-03; Osborne)

60 APPLIED LIFE SCIENCES↗
DOE OSTI2015

SU-E-I-82: PET Radiopharmaceuticals for Prostate Cancer Imaging: A Review

Purpose: The aim of this work was to review new and clinical practice PET radiopharmaceuticals for prostate cancer imaging. Methods: PET radiopharmaceuticals were reviewed on the main databases. Availability, dosimetry, accuracy and limitations were considered. Results: The following radioisotopes with respective physical half-life and mean positron energy were found: {sup 18}F (109,7 min, 249,8 keV), {sup 89}Zr (78,4 hs, 395,5 keV), {sup 11}C (20,4 min, 385,7 keV) and {sup 68}Ga (67,8 min, 836 keV). {sup 68}Ga was the only one not produced by cyclotron. Radiopharmaceuticals uptake by glucose metabolism ({sup 18}F-FDG), lipogenesis ({sup 11}C-Choline and {sup 11}C-Acetate), amino acid transport (Anti-{sup 18}F-FACBC), bone matrix ({sup 18}F-NaF), prostatespecific membrane antigen ({sup 68}Ga-PSMA and {sup 89}Zr-J591), CXCR receptors ({sup 89}Ga-Pentixafor), adrenal receptors ({sup 18}F-FDHT) and gastrin release peptide receptor (bombesin analogue). Most of radiopharmaceuticals are urinary excretion, so bladder is the critical organ. 11C-choline (pancreas), Anti-{sup 18}FFACBC (liver) and {sup 18}F-FBDC (stomach wall) are the exception. Higher effective dose was seen {sup 18}F-NaF (27 μSv/MBq) while the lowest was {sup 11}CAcetate (3,5 μSv/MBq). Conclusion: Even though {sup 18}F-FDG has a large availability its high urinary excretion and poor uptake to slow growing disease offers weak results for prostate cancer. Better accuracy is obtained when {sup 18}F-NaF is used for bone metastatic investigation although physicians tend to choose bone scintigraphy probably due to its cost and practice. Many guidelines in oncology consider {sup 11}C or {sup 18}F labeled with Choline the gold standard for biochemical relapse after radical treatment. Local, lymph node and distant metastatic relapse can be evaluated at same time with this radiopharmaceutical. There is no consensus over bigger urinary excretion for {sup 18}F labeling. Anti-{sup 18}F-FACBC, {sup 68}Ga-PSMA and {sup 68}Ga-Pentixafor are demonstrating good results but more researches are needed. While PSMA imaging seems to be independent of PSA level, one choline limitation, anti-{sup 18}F-FACBC adds value because imaging any disease stage. {sup 68}Ga-Petixafor is being tested as theranostics marker integrating molecular image and therapy.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2024

Development of 52Mn Labeled Trastuzumab for Extended Time Point PET Imaging of HER2

Abstract Purpose Due to their long circulation time in the blood, monoclonal antibodies (mAbs) such as trastuzumab, are usually radiolabeled with long-lived positron emitters for the development of agents for Positron Emission Tomography (PET) imaging. Manganese-52 ( 52 Mn, t 1/2 = 5.6 d, β + = 29.6%, E(β ave ) = 242 keV) is suitable for imaging at longer time points providing a complementary technique to Zirconium-89 ( 89 Zr, t 1/2 = 3.3 d, β + = 22.7%, E(β ave ) = 396 keV)) because of its long half-life and low positron energy. To exploit these properties, we aimed to investigate suitable bifunctional chelators that could be readily conjugated to antibodies and labeled with 52 Mn under mild conditions using trastuzumab as a proof-of-concept. Procedures Trastuzumab was incubated with S-2-(4-isothiocyanatobenzyl)-1,4,7,10-tetraazacyclododecane tetraacetic acid (p-SCN-Bn-DOTA), 1-Oxa-4,7,10-tetraazacyclododecane-5-S-(4-isothiocyantobenzyl)-4,7,10-triacetic acid (p-SCN-Bn-Oxo-DO3A), and 3,6,9,15-tetraazabicyclo[9.3.1] pentadeca-1(15),11,13-triene-4-S-(4-isothiocyanatobenzyl)-3,6,9-triacetic acid (p-SCN-Bn-PCTA) at a tenfold molar excess. The immunoconjugates were purified, combined with [ 52 Mn]MnCl 2 at different ratios, and the labeling efficiency was assessed by iTLC. The immunoreactive fraction of the radiocomplex was determined through a Lindmo assay. Cell studies were conducted in HER2 + (BT474) and HER2- (MDA-MB-468) cell lines followed by in vivo studies. Results Trastuzumab-Oxo-DO3A was labeled within 30 min at 37 °C with a radiochemical yield (RCY) of 90 ± 1.5% and with the highest specific activity of the chelators investigated of 16.64 MBq/nmol. The labeled compound was purified with a resulting radiochemical purity of > 98% and retained a 67 ± 1.2% immunoreactivity. DOTA and PCTA immunoconjugates resulted in < 50 ± 2.5% (RCY) with similar specific activity. Mouse serum stability studies of [ 52 Mn]Mn-Oxo-DO3A-trastuzumab showed 95% intact complex for over 5 days. Cell uptake studies showed higher uptake in HER2 + (12.51 ± 0.83% /mg) cells compared to HER2- (0.85 ± 0.10%/mg) cells. PET images of mice bearing BT474 tumors showed high tumor uptake that was consistent with the biodistribution (42.02 ± 2.16%ID/g, 14 d) compared to MDA-MB-468 tumors (2.20 ± 0.80%ID/g, 14 d). Additionally, both models exhibited low bone uptake of < 1% ID/g. Conclusion The bifunctional chelator p-SCN-Bn-Oxo-DO3A is promising for the development of 52 Mn radiopharmaceuticals as it was easily conjugated, radiolabeled at mild conditions, and illustrated stability for a prolonged duration both in vitro and in vivo . High-quality PET/CT images of [ 52 Mn]Mn-Oxo-DO3A-trastuzumab were obtained 14 d post-injection. This study illustrates the potential of [ 52 Mn]Mn-Oxo-DO3A for the evaluation of antibodies using PET imaging.

Omweri, James M.↗
DOE OSTI2014

Di-macrocyclic terephthalamide ligands as chelators for the PET radionuclide zirconium-89

The development of bifunctional chelators (BFCs) which can stably chelate zirconium-89 ((89)Zr) while being conjugated to targeting molecules is an area of active research. Herein we report the first octadentate terephthalamide ligands, which are easily radiolabeled with (89)Zr and are highly stable in vitro. Lastly, they represent a novel class of chelators, which are worthy of further development as BFCs for (89)Zr.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

s-processing in AGB stars revisited. I. Does the main component constrain the neutron source in the {sup 13}C pocket?

Slow neutron captures at A ≳ 85 are mainly guaranteed by the reaction {sup 13}C(α,n){sup 16}O in asymptotic giant branch (AGB) stars, requiring proton injections from the envelope. These were so far assumed to involve a small mass (≲ 10{sup –3} M {sub ☉}), but models with rotation suggest that in such tiny layers excessive {sup 14}N hampers s-processing. Furthermore, s-element abundances in galaxies require {sup 13}C-rich layers substantially extended in mass (≳ 4 × 10{sup –3} M {sub ☉}). We therefore present new calculations aimed at clarifying those issues and at understanding whether the solar composition helps to constrain the {sup 13}C 'pocket' extension. We show that: (1) mixing 'from bottom to top' (as in magnetic buoyancy or other forced mechanisms) can form a {sup 13}C reservoir substantially larger than assumed so far, covering most of the He-rich layers; (2) on the basis of this idea, stellar models at a fixed metallicity reproduce the main s-component as accurately as before; and (3) they make nuclear contributions from unknown nucleosynthesis processes (LEPP) unnecessary, against common assumptions. These models also avoid problems of mixing at the envelope border and fulfil requirements from C-star luminosities. They yield a large production of nuclei below A = 100, so that {sup 86,} {sup 87}Sr may be fully synthesized by AGB stars, while {sup 88}Sr, {sup 89}Y, and {sup 94}Zr are contributed more efficiently than before. Finally, we suggest tests suitable for providing a final answer regarding the extension of the {sup 13}C pocket.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2014

Production of Positron Emitting Radiometals: Cu-64, Y-86, Zr-89. Final report

This proposal seeks support to increase our production of the radionuclides yttrium-86 and zirconium-89 while continuing to produce copper-64. We have the advantage that we already ship out copper-64 to some 20-25 institutions per week (over 60 different institutions total including 4 Canadian sites) and thus our group already has significant experience with producing, purifying and shipping radioactive materials. A significant portion of the funds requested supported the purchase of a new hotcell for the production of zirconium-89 and yttrium-86.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2017

Excitation Function Calculations of Neutron-Induced Reactions of Some Zirconium Target Isotopes

Nuclear structures with high performance materials will be critical for the success of future fusion energy. Zirconium alloys are extensively used for nuclear reactor core materials as fuel cladding and guide tubes due to excellent radiation and corrosion resistant properties. In this paper, the excitation functions of {sup 90}Zr(n,2n){sup 89}Zr, {sup 90}Zr(n,α){sup 87}Sr, {sup 91}Zr(n,p){sup 91}Y and {sup 92}Zr(n,p){sup 92}Y nuclear reactions were calculated for energies up to 25 MeV. Besides, ALICE/ASH and TALYS 1.6 codes were used for the cross section calculations. The obtained calculations were compared with the experimental data in the literature.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2013

Radiative strength functions for dipole transitions in {sup 90}Zr

Partial cross sections for the (p, {gamma}) reaction on the {sup 89}Y nucleus that were measured previously at proton energies between 2.17 and 5.00 MeV and which were averaged over resonances were used to determine the absolute values and the energy distribution of the strength of dipole transitions from compound-nucleus states to low-lying levels of the {sup 90}Zr nucleus. The data obtained in this way were compared with the predictions of various models.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Nuclear activation analysis of zirconium-90 isomeric and ground-state reactions at the OMEGA Laser Facility

Nuclear activation is a well-established technique for inferring neutron yields in laser direct-drive deuterium–tritium (DT) and deuterium–deuterium (D 2 ) implosions at the OMEGA Laser Facility. Zirconium has long been considered an excellent candidate for measuring DT neutron fusion yields by observing decays of the 90 Zr(n,2n) 89 Zr ground-state reaction. As it has a higher energy threshold than present activation detectors utilizing copper, zirconium provides a means to infer primary neutron yields that are less susceptible to being skewed due to neutron scattering within the experimental environment. However, with a 78.41-h half-life, it is not operationally practical to utilize this reaction for OMEGA experiments, which have a 1-h shot cycle. Zirconium’s 90 Zr(n,2n) 89 mZr reaction presents itself as a viable candidate to infer neutron yields within a shot cycle, given its half-life of 4.16 min. Here, we present an overview of the approach and methodology, utilizing first principles techniques, to infer the primary neutron yields from OMEGA DT fusion experiments by using both the isomeric and the ground-state reaction. Yields inferred from both reactions are compared, which are in good agreement between the two.

Activation analysis↗
DOE OSTI2017

Evaluation of macrocyclic hydroxyisophthalamide ligands as chelators for zirconium-89

The development of bifunctional chelators (BFCs) for zirconium-89 immuno-PET applications is an area of active research. We report the synthesis and evaluation of octadentate hydroxyisophthalamide ligands (1 and 2) as zirconium-89 chelators. And while both radiometal complexes could be prepared quantitatively and with excellent specific activity, preparation of 89 Zr-1 required elevated temperature and an increased reaction time. 89 Zr-1 was more stable than 89 Zr-2 when challenged in vitro by excess DTPA or serum proteins and in vivo during acute biodistribution studies. The differences in radiometal complex stability arise from structural changes between the two ligand systems, and suggest further ligand optimization is necessary to enhance 89 Zr chelation.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2018

Tandem column isolation of zirconium-89 from cyclotron bombarded yttrium targets using an automated fluidic platform: Anion exchange to hydroxamate resin columns

The development of a tandem column purification method for the production of high-purity 89Zr is presented. The primary column was a macroporous strongly basic anion exchange resin on styrene divinylbenzene co-polymer. The secondary column, with an internal volume of ~27 µL, was packed with hydroxamate resin. A condition of inverted selectivity was developed, whereby the 89Zr eluent from the primary column is synonymous with the load condition on the secondary column. The ability to transfer 89Zr from one column to the next allows two sequential column clean-up methods to be performed prior to the final elution of the 89Zr. This approach assures delivery of high purity 89Zr product and assures a 89Zr product that is eluted in a substantially smaller volume than is possible when using the traditionally-employed single hydroxamate resin column method. The tandem column purification process has been implemented into a prototype automated fluidic system. The system is configured with on-line gamma detection so column effluents can be monitored in near-real time. The automated method was tested using seven cyclotron bombarded Y foil targets. It was found that 95.1±1.3% of the 89Zr present in the foils was recovered in the secondary column elution fraction. Furthermore, elution peak analysis of several 89Zr elution profile radiochromatograms made possible the determination of 89Zr recovery as a function of volume; a 89Zr product volume that contains 90% of the mean secondary column elution peak can be obtained in 0.29±0.06 mL (representing 86±5% of the 89Zr activity in the target). This product volume represents a significant increase in isotope product concentration over the predominant method used in the field. In addition to the reduced 89Zr product elution volume, titrations of the 89Zr product with deferoxamine mesylate salt across two preparatory methods resulted in mean effective specific activity (ESA) values of 279 and 340 TBq·mmole-1 and mean bindable metals concentrations ([MB]) of 13.5 and 16.7 nmole·g-1. These ESA and [MB] values infer that the 89Zr product resulting from this tandem column isolation method has the highest purity reported to date.

immunoPET, zirconium-89, laboratory automation, de↗