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All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Nuclear Data Sheets for A = 227

The evaluated spectroscopic data are presented for ten known nuclides of mass 227 (Po, At, Rn, Fr, Ra, Ac, Th, Pa, U, Np). For {sup 227}Po, {sup 227}At, {sup 227}Rn, {sup 227}Pa, {sup 227}U and {sup 227}Np nuclei, only the ground-state information is available. Their decay characteristics are mostly unknown. Levels in {sup 227}Fr are known only from the decay of {sup 227}Rn to {sup 227}Fr. This decay scheme at present cannot be normalized to deduce γ intensities per 100 decays due to lack of knowledge about multipolarities of many low-energy transitions. The levels in {sup 227}Ra, {sup 227}Ac and {sup 227}Th are known from several decays and reactions, including particle-transfer data for {sup 227}Ra and {sup 227}Ac. The decay scheme of {sup 227}Ra to {sup 227}Ac was last studied in 1971 using small Ge detectors. Improved γ-ray intensity data need to be obtained with a better γ-detection system. The datasets for {sup 227}Ac have undergone extensive revisions, including detailed data for 231Pa α decay from 1986BaYK report, and single-proton transfer data from 1986MaYU thesis. High-spin (J>13/2 or so) structures are known only for 227Th. Level lifetime data are quite scarce for all the nuclides in this mass chain, thus limiting the knowledge of reduced transition probabilities. Band structures for {sup 227}Fr, {sup 227}Ra, {sup 227}Ac and {sup 227}Th are known in detail, together with evidence of weak octupole deformation and consequent parity-doublet structures. This evaluation was carried out as part of a joint IAEA-ICTP workshop for Nuclear Structure and Decay Data, organized and hosted by the IAEA, Vienna and ICTP, Trieste, March 24–28, 2014. The evaluation work was coordinated by B. Singh (McMaster). This work supersedes previous A=227 evaluation (2001Br31) published by E. Browne which covered literature before May 2001.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2019

Recommended Nuclear Data for the Production of Selected Therapeutic Radionuclides

Increasing interest in the treatment of human disease by means of targeted radionuclide-based therapies requires an accurate understanding of achievable yields and quantification of realisable degrees of purity. Important studies within a more extensive Coordinated Research Project of the International Atomic Energy Agency (IAEA CRP) have included in-depth assessments and evaluations of all available measured cross-section data for ten nuclear reactions leading to the formation of 131 Cs, 131 Ba, 225 Ac, 225 Ra, 227 Th, 227 Ac, 230 U and 230 Pa for various on-going and proposed therapeutic applications in nuclear medicine. Equivalent studies were also undertaken of possible reactions to produce the 178W /low-spin 178m Ta generator system that has been clinically applied in diagnosis by means of SPECT - these particular cross-section studies and recommendations are included in this paper for completeness. All available measured data have been critically reviewed and assessed to produce statistically consistent datasets. Selected datasets have been fitted by a least-squares method with Padé approximations of variable order to evaluate the production cross sections and corresponding uncertainties. New measurements have been made in some instances, and reported data have been adjusted to accommodate new nuclear decay or monitor reaction data which altered the original reported quantities adversely. Insufficient measured data are available in many cases to permit a reliable evaluation of cross sections, and these instances are discussed. Finally, recommended therapeutic radionuclide production reaction data and their uncertainties are available on the Web page of the IAEA Nuclear Data Section at www-nds.iaea.org/radionuclides/ and also at the IAEA medical portal www-nds.iaea.org/medportal/.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
DOE OSTI2019

A Method for Understanding the Behaviour of Radioactive Decay Chains in Radiological Assessments - 19382

In many radiological groundwater pathway assessments, especially those where the assessment timescales of interest are relatively short (say a few thousand years or less), contributions to effective dose or radiological risk are dominated by radionuclides such as C-14, Cl-36 or I-129. Over longer timescales, additional radionuclides can also become key contributors to risk. In particular, members of the U-238 decay chain, notably Ra-226 and Pb-210, are likely to be key radionuclides. Other decay chains that can contribute significantly to dose or risk at times far into the future include Np-237 → U-233 → Th-229 and U-235 → Pa-231 → Ac-227. In this paper, a method is described for understanding decay chain behaviour in radiological assessments. The method uses a graphical approach in which the various modes of transport and decay in a system of connected compartments are represented as pathways between two nodes in a two-dimensional grid. Each pathway corresponds to a distinct transport and decay process. By so doing, the different transport and decay processes can be identified in a systematic way. The result is an algorithm for generating the contributions to effective dose or radiological risk without explicit solution of the transport equations. The method has been tested against numerical models and analytic solutions and found to give excellent agreement, while at the same time providing information about decay chain behaviour that would be difficult to obtain from a numerical assessment model. The power of the method is illustrated by applying it to some examples based on real repository concepts. (authors)

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2020

The HRA/Solarium Project: Feedback Based on 20 Years of Experience in Treatment of Medium Level Waste - 20185

Since the 1980's the management of the historical site of Mol has been transferred to the National Agency for Radioactive Waste and Enriched Fissile Materials (ONDRAF/NIRAS). Belgoprocess is entrusted by ONDRAF/NIRAS with the operational waste management and site remediation. One of the major challenges has been the characterization, treatment and conditioning of approximately 200 m{sup 3} of medium level waste. These waste packages were stored in poor conditions in storage vaults ('HRA') or concrete containers ('Solarium'). They have been produced in various research programs and reactor operations at the Belgian nuclear energy research centre SCK.CEN, isotope production, decontamination and dismantling operations from the 1960's up to the 1980's. Despite the limited volume, this historical waste consists of a great variation of waste characteristics and waste configurations. To tackle these liabilities, a new processing facility was built in the 1990's to allow safe transfers, handling, characterization and treatment of these packages. Also some auxiliary facilities have been built to deal with the by-products, like emptied concrete containers. The engineering of the installation, safety procedures and (characterization) methodology that has been developed generically have been proved to be successful. Nevertheless, the specific nature of some items made it necessary to organize a step-by-step treatment in distinct campaigns in which some relevant extra (safety) measures had to be taken into account. This dynamic approach made it possible to process a great variety of waste types in order to to ensure that this legacy is no longer left for subsequent generations. After about 20 years of operations, there has been a great build-up of experience and feed-back concerning the waste management of these specific waste streams. Some cases will be highlighted to specify the approach followed for treatment of e.g.: - Na/NaK containing equipment; - spent radioactive sources; - fuel element residues; - medium level waste originating from activation experiments; - radium bearing medium level waste originating from Ac-227 production research. (authors)

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2017

Synthesis and Characterization of the Actinium Aquo Ion

Metal aquo ions occupy central roles in all equilibria that define metal complexation in natural environments. These complexes are used to establish thermodynamic metrics (i.e., stability constants) for predicting metal binding, which are essential for defining critical parameters associated with aqueous speciation, metal chelation, in vivo transport, and so on. As such, establishing the fundamental chemistry of the actinium(III) aquo ion (Ac-aquo ion, Ac(H 2 O) x 3+ ) is critical for current efforts to develop 225 Ac [t 1/2 = 10.0(1) d] as a targeted anticancer therapeutic agent. However, given the limited amount of actinium available for study and its high radioactivity, many aspects of actinium chemistry remain poorly defined. We overcame these challenges using the longer-lived 227 Ac [t 1/2 = 21.772(3) y] isotope and report the first characterization of this fundamentally important Ac-aquo coordination complex. Our X-ray absorption fine structure study revealed 10.9 ± 0.5 water molecules directly coordinated to the Ac III cation with an Ac–O H2O distance of 2.63(1) Å. This experimentally determined distance was consistent with molecular dynamics density functional theory results that showed (over the course of 8 ps) that Ac III was coordinated by 9 water molecules with Ac–O H2O distances ranging from 2.61 to 2.76 Å. Lastly, the data is presented in the context of other actinide(III) and lanthanide(III) aquo ions characterized by XAFS and highlights the uniqueness of the large Ac III coordination numbers and long Ac–O H2O bond distances.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Examination of Ac-225 production from Ra-226 using fast reactor JOYO

In this study, the authors investigated the method of producing the radionuclide Ac{sup 225} used for targeted alpha therapy (TAT). Currently, Ac{sup 225} is mainly generated from ORNL's Th{sup 229} generator, and the annual production amount is limited to about 63 GBq, and methods for generating it using accelerators are under development in each country. The method using an accelerator has the advantage of being able to generate Ac{sup 225} from a small amount of target nuclides with high efficiency but has the disadvantage of not being able to irradiate a large amount of target nuclides at once due to the small irradiation area. Therefore, the authors investigated a method to generate Ac{sup 225} by neutron irradiation of Ra{sup 226} as a target nuclide using the experimental fast reactor JOYO, which has abundant neutrons and a large loading region. Irradiation of Ra{sup 226} with fast neutrons causes a (n, 2n) reaction to generate Ra{sup 225}, and then decay to produce Ac{sup 225}. In addition, although harmful Ac{sup 227} is also produced at the same time by the (n,γ) reaction, first of all the actinium isotope is chemically separated and eliminated. Since the remaining Ra{sup 225} collapses and Ac{sup 225} is produced, pure Ac{sup 225} can be extracted by performing chemical separation again. As a result of the analysis, 1 g of Ra{sup 226} is irradiated with JOYO for 60 days, and milking is performed 4 times every 17.5 days. By doing these three times a year, it was found that about 50 GBq of Ac{sup 225} was generated. (authors)

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2019

The application of poorly crystalline silicotitanate in production of 225 Ac

Actinium-225 ( 225 Ac) can be produced from a Thorium-229/Radium-225 ( 229 Th/ 225 Ra) generator, from high/low energy proton irradiated natural Thorium or Radium-226 target. Titanium based ion exchanger were evaluated for purification of 225 Ac. Poorly crystalline silicotitanate (PCST) ion exchanger had high selectivity for Ba, Ag and Th. 225 Ac was received with trace amounts of 227 Ac, 227 Th and 223 Ra, and the solution was used to evaluate the retention of the isotopes on PCST ion exchanger. Over 90% of the 225 Ac was recovered from PCST, and the radiopurity was >99% (calculated based on 225 Ac, 227 Th, and 223 Ra). The capacity of the PCST inorganic ion exchange for Barium and 232 Th was determined to be 24.19 mg/mL for Barium and 5.05 mg/mL for Thorium. PCST ion exchanger could separate 225 Ac from isotopes of Ra and Th, and the process represents an interesting one step separation that could be used in an 225 Ac generator from 225 Ra and/or 229 Th. Capacity studies indicated PCST could be used to separate 225 Ac produced on small 226 Ra targets (0.3–1 g), but PCST did not have a high enough capacity for production scale Th targets (50–100 g).

43 PARTICLE ACCELERATORS↗
DOE OSTI2016

Reactor production of Thorium-229

Limited availability of 229 Th for clinical applications of 213 Bi necessitates investigation of alternative production routes. In reactor production, 229 Th is produced from neutron transmutation of 226 Ra, 228 Ra, 227 Ac and 228 Th. Here, we evaluate irradiations of 226 Ra, 228 Ra, and 227 Ac targets at the ORNL High Flux Isotope Reactor.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2016

Pulse-shape discrimination and energy quenching of alpha particles in Cs 2 LiLaBr 6 :Ce 3+

Cs 2 LiLaBr 6 :Ce 3+ (CLLB) is an elpasolite scintillator that offers excellent linearity and gamma-ray energy resolution and sensitivity to thermal neutrons with the ability to perform pulse-shape discrimination (PSD) to distinguish gammas and neutrons. Our investigation of CLLB has indicated the presence of intrinsic radioactive alpha background that we have determined to be from actinium contamination of the lanthanum component. We measured the pulse shapes for gamma, thermal neutron, and alpha events and determined that PSD can be performed to separate the alpha background with a moderate figure of merit of 0.98. Here, we also measured the electron-equivalent-energy of the alpha particles in CLLB and simulated the intrinsic alpha background from 227 Ac to determine the quenching factor of the alphas.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Actinium chelation and crystallization in a macromolecular scaffold

Abstract Targeted alpha therapy (TAT) pairs the specificity of antigen targeting with the lethality of alpha particles to eradicate cancerous cells. Actinium-225 [ 225 Ac; t 1/2 = 9.920(3) days] is an alpha-emitting radioisotope driving the next generation of TAT radiopharmaceuticals. Despite promising clinical results, a fundamental understanding of Ac coordination chemistry lags behind the rest of the Periodic Table due to its limited availability, lack of stable isotopes, and inadequate systems poised to probe the chemical behavior of this radionuclide. In this work, we demonstrate a platform that combines an 8-coordinate synthetic ligand and a mammalian protein to characterize the solution and solid-state behavior of the longest-lived Ac isotope, 227 Ac [t 1/2 = 21.772(3) years]. We expect these results to direct renewed efforts for 225 Ac-TAT development, aid in understanding Ac coordination behavior relative to other +3 lanthanides and actinides, and more broadly inform this element’s position on the Periodic Table.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Measurement of 227 Ac impurity in 225 Ac using decay energy spectroscopy

225 Ac is a valuable medical radionuclide for targeted $\alpha$ therapy, but 227 Ac is an undesirable byproduct of an accelerator-based synthesis method under investigation. Sufficient detector sensitivity is critical for quantifying the trace impurity of 227 Ac, with the 227 Ac/ 225 Ac activity ratio predicted to be approximately 0.15% by end-of-bombardment (EOB). Superconducting transition edge sensor (TES) microcalorimeters offer high resolution energy spectroscopy using the normal-to-superconducting phase transition to measure small changes in temperature. By embedding 225 Ac production samples in a gold foil thermally coupled to a TES microcalorimeter we can measure the decay energies of the radionuclides embedded with high resolution and 100% detection efficiency. This technique, known as decay energy spectroscopy (DES), collapses several peaks from $\alpha$ decays into single Q-value peaks. In practice there are more complex factors in the interpretation of data using DES, which we will discuss in this paper. Using this technique we measured the EOB 227 Ac impurity to be (0.142 ± 0.005)% for a single production sample. This demonstration has shown that DES is a useful tool for quantitative measurements of complicated spectra.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2022

Evaluation of 134 Ce as a PET imaging surrogate for antibody drug conjugates incorporating 225 Ac

The in vivo generator 134 Ce/ 134 La has the potential to serve as a PET imaging surrogate for both alpha-emitting 225 Ac and 227 Th radionuclides due to the unique Ce III /Ce IV redox couple and the relatively long half-life of 134 Ce. Furthermore, the purpose of this study was to demonstrate the compatibility of 134 Ce with DOTA-based antibody drug conjugates, which would act as therapeutic agents when incorporating 225 Ac.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2019

Gadolinium vanadate nanocrystals as carriers of α-emitters ( 225 Ac, 227 Th) and contrast agents

Gadolinium vanadate (GdVO 4 ) core and core +2 shell nanocrystals (NCs) were evaluated for in vitro retention of 225 Ac, 227 Th, and their first decay daughters, 221 Fr and 223 Ra, respectively. GdVO 4 NCs with a tetragonal crystal system (zircon-type) and spherical morphology were obtained by precipitation of GdCl 3 and Na 3 VO 4 using sodium citrate as a complexing agent. The growth of two nonradioactive GdVO 4 shells on both Gd( 225 Ac)VO 4 and Gd( 227 Th)VO 4 core NCs was demonstrated by an increase of 0.7 nm and 2 nm in the crystallite size, respectively. The maximum leakage of 225 Ac was 15% and 2.4% from core and core + 2 shells, whereas the leakage of 227 Th was 3% and 1.5%, respectively. The presence of two nonradioactive GdVO 4 shells increased the retention of 221 Fr and 223 Ra by 20% and 15% with respect to core NCs. Furthermore, a longitudinal proton relaxivity, r 1 = 0.9289 s –1 mM –1 , confirmed their potential application as contrast agents for magnetic resonance imaging. In summary, GdVO 4 NCs show promising capabilities as radionuclide carriers with partial retention of decay daughters and as contrast agents for theranostic applications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Transport model predictions of 225 Ac production cross sections via energetic p, d and α irradiation of 232 Th targets

Monte Carlo transport codes PHITS and MCNP6 were used to calculate the production cross sections of 225,227 Ac, 227,229 Th, 223,225 Ra, and 229,230,231 Pa via the bombardment of a 232 Th target with energetic protons, deuterons, and α-particles. The incident projectile energies ranged between 10 and 800 MeV/nucleon. When possible, the predicted production cross sections were compared with the available experimental data and other predictions. Here, the degree of the codes’ abilities to match the measured data provides a qualitative assessment of the codes’ abilities to predict data from similar, but unmeasured, projectile/target systems. In addition, a comparison between calculated cross sections and data may provide insight into possible improvements in the physics models employed by those transport codes.

223Ra↗