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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Krypton-85 chronometry of spent nuclear fuel

We describe the use of the radionuclide 85 Kr, which is produced by nuclear fission and has a half-life of 10.76 years, to determine the age of spent nuclear fuel. The method is based on mass-spectrometric measurement of the relative abundance of fissiogenic Kr isotopes extracted from a fuel sample, and we show that it can be applied to micron-scale particles of spent fuel that are analogous to particles that have been released into the environment from various nuclear facilities in the past. 85 Kr chronometry is potentially valuable for identifying and attributing nuclear materials, grouping samples into collections of common origin that can be used to reconstruct the origin and irradiation history of the material, and verifying declared nuclear activities in the context of international monitoring programs.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

First experimental determination of the ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar reaction cross section and ³⁹Ar production in Earth’s atmosphere

The cosmogenic ³⁹Ar(t1∕2 = 268 years) isotope of argon is used for geophysical dating and tracing of underground and ocean water, as well as ice owing to its appropriate half-life and chemical inertness as a noble gas; ³⁹Ar serves also in nuclear weapon test monitoring. We measured for the first time the total cross section of the main ³⁹Ar cosmogenic production reaction in the atmosphere, namely ⁴⁰Ar(𝑛, 2𝑛)39 Ar, using 14.8 ± 0.3 MeV neutrons. The neutrons, produced by a deuterium-tritium generator, impinged on a stainless steel sphere filled with Ar gas highly enriched in the ⁴⁰Ar isotope and were monitored by a stack of fast-neutron activation foils. The reaction yield was measured by atom counting of long-lived ³⁹Ar with noble gas accelerator mass spectrometry and, independently, by decay counting relative to atmospheric argon (³⁹Ar/Ar= 8.12 × 10−16 ). A total ⁴⁰Ar(𝑛, 2𝑛)39 Ar cross section of 610 ± 100 mb was determined at 14.8 ± 0.3 MeV incident neutron energy. This result serves as a benchmark for recent theoretical calculations and evaluations, found to reproduce well the experimental total cross section. We use these energy-dependent theoretical cross sections together with experimental spectra of cosmogenic neutrons at different altitudes to calculate the global average rate of neutron-induced ³⁹Ar atmospheric production, resulting in 770 ± 240 39 Ar atoms/cm²/day. The secular equilibrium between the ³⁹Ar calculated production rate and radioactive decay rate leads to a partial isotopic abundance ³⁹Ar/Ar = (5.9 ± 1.8) × 10−16 , showing that ≈73% of atmospheric ³⁹Ar is produced by cosmogenic neutrons, the remaining part believed to be induced by muons and high-energy 𝛾 rays. The ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar cross section at 14 MeV is also a key parameter for quantifying the anthropogenic contribution to atmospheric 39 Ar produced during the thermonuclear tests of the 1960s. We estimate that anthropogenic ³⁹Ar accounts for roughly 20% of the present atmospheric inventory.

39 Ar atmospheric production↗
DOE OSTI2024

Development of CD46 targeted alpha theranostics in prostate cancer using 134 Ce/ 225 Ac-Macropa-PEG 4 -YS5

Rationale: 225 Ac, a long-lived α-emitter with a half-life of 9.92 days, has garnered significant attention as a therapeutic radionuclide when coupled with monoclonal antibodies and other targeting vectors. Nevertheless, its clinical utility has been hampered by potential off-target toxicity, a lack of optimized chelators for 225 Ac, and limitations in radiolabeling methods. In a prior study evaluating the effectiveness of CD46-targeted radioimmunotherapy, we found great therapeutic efficacy but also significant toxicity at higher doses. To address these challenges, we have developed a radioimmunoconjugate called 225 Ac-Macropa-PEG 4 -YS5, incorporating a stable PEGylated linker to maximize tumoral uptake and increase tumor-to-background ratios. Our research demonstrates that this conjugate exhibits greater anti-tumor efficacy while minimizing toxicity in prostate cancer 22Rv1 tumors. Methods: We synthesized Macropa.NCS and Macropa-PEG 4/8 -TFP esters and prepared Macropa-PEG 0/4/8 -YS5 (with nearly ~1:1 ratio of macropa chelator to antibody YS5) as well as DOTA-YS5 conjugates. These conjugates were then radiolabeled with 225 Ac in a 2 M NH 4 OAc solution at 30 °C, followed by purification using YM30K centrifugal purification. Subsequently, we conducted biodistribution studies and evaluated antitumor activity in nude mice (nu/nu) bearing prostate 22Rv1 xenografts in both single-dose and fractionated dosing studies. Micro-PET imaging studies were performed with 134 Ce-Macropa-PEG 0/4/8 -YS5 in 22Rv1 xenografts for 7 days. Toxicity studies were also performed in healthy athymic nude mice. Results: As expected, we achieved a >95% radiochemical yield when labeling Macropa-PEG 0/4/8 -YS5 with 225 Ac, regardless of the chelator ratios (ranging from 1 to 7.76 per YS5 antibody). The isolated yield exceeded 60% after purification. Such high conversions were not observed with the DOTA-YS5 conjugate, even at a higher ratio of 8.5 chelators per antibody (RCY of 83%, an isolated yield of 40%). Biodistribution analysis at 7 days post-injection revealed higher tumor uptake for the 225 Ac-Macropa-PEG 4 -YS5 (82.82 ± 38.27 %ID/g) compared to other conjugates, namely 225 Ac-Macropa-PEG 0/8 -YS5 (38.2 ± 14.4/36.39 ± 12.4 %ID/g) and 225 Ac-DOTA-YS5 (29.35 ± 7.76 %ID/g). The PET Imaging of 134 Ce-Macropa-PEG 0/4/8 -YS5 conjugates resulted in a high tumor uptake, and tumor to background ratios. In terms of antitumor activity, 225 Ac-Macropa-PEG 4 -YS5 exhibited a substantial response, leading to prolonged survival compared to 225 Ac-DOTA-YS5, particularly when administered at 4.625 kBq doses, in single or fractionated dose regimens. Chronic toxicity studies observed mild to moderate renal toxicity at 4.625 and 9.25 kBq doses. Conclusions: Our study highlights the promise of 225 Ac-Macropa-PEG 4 -YS5 for targeted alpha particle therapy. The 225 Ac-Macropa-PEG 4 -YS5 conjugate demonstrates improved biodistribution, reduced off-target binding, and enhanced therapeutic efficacy, particularly at lower doses, compared to 225 Ac-DOTA-YS5. Incorporating theranostic 134 Ce PET imaging further enhances the versatility of macropa-PEG conjugates, offering a more effective and safer approach to cancer treatment. Overall, this methodology has a high potential for broader clinical applications.

60 APPLIED LIFE SCIENCES↗
NASA NTRS1972

Radiation from plutonium 238 used in space applications

The principal mode of the nuclear decay of plutonium 238 is by alpha particle emission at a rate of 17 curies per gram. Gamma radiation also present in nuclear fuels arises primarily from the nuclear de-excitation of daughter nuclei as a result of the alpha decay of plutonium 238 and reactor-produced impurities. Plutonium 238 has a spontaneous fission half life of 4.8 x 10 to the 10th power years. Neutrons associated with this spontaneous fission are emitted at a rate of 28,000 neutrons per second per gram. Since the space fuel form of plutonium 238 is the oxide pressed into a cermet with molybdenum, a contribution to the neutron emission rate arises from (alpha, n) reactions with 0-17 and 0-18 which occur in natural oxygen.

Keenan, T. K.↗
NASA NTRS1972

Developable images produced by x-rays using the nickel-hypophosphite system. 2: Exposure and development parameters for sodium hypophosphite

Crystalline sodium hypophosphite was X-irradiated and then treated with an ammoniacal nickel hypophosphite solution. Treatment resulted in the precipitation of nickel metal. The yield of nickel metal varied directly with particle size, sample weight, X-ray voltage, target current, exposure time, and development time. These findings show the process to be potentially useful in X-ray type photography. The half-life for the latent image species was found to be relatively short; but this is not critical in most X-ray photography applications. Furthermore, the work can be interpreted on the basis that a hydrogen atom is involved in the mechanism and indicates that the autocatalytic development step may be self-poisoning.

May, C. E.↗
NASA NTRS1972

Equatorial electron energy and number densities in the Jovian magnetosphere

A synchrotron model with a Maxwellian energy distribution of the form e to the (-E/E sub 0) power is used in a comparison with spatially resolved radio interferometric measurements of the Jovian emission. The observations of the decimeter radiation as a function of equatorial distance at 10.4 and 21 cm wavelength were reduced to source emission/cc of source electrons in each of 16 concentric rings. The peak energies for isotropically distributed electrons exceeded the maximum energy for flat orbiting electrons, and the peaks were generally located from 2.25 to 3 Jupiter radii. Beyond 3 radii, the order of magnitude on number density became a sensitive function of pitch angle distribution. The total equatorial intensities at 75 cm wavelength were computed for (E sub 0)(r) and n(r) at different values of B sub 0. The radiative half life for electrons of initial energy E sub 0 in a dipole field was calculated and found to be nearly constant at one year or less for altitudes at and below the position in peak energy.

Luthey, J. L.↗
NASA NTRS1972

Technique for rapid determination of relative ages of lunar areas from orbital photography.

Development of a technique for determining relative ages of regions of the lunar surface from orbital photography using a model of small-impact erosion. The erosion model relates the shape of a crater to the integrated flux of debris that has impacted the surface since that crater was fresh. The shape of the most modified crater of a particular diameter is thereby related to the relative age of the surface. Application of this analysis to orbital photography reveals that the major mare units vary in the accumulation of impacts by more than a factor of 3. Comparison of these data with crystallization ages determined from samples collected during the Apollo 11 and 12 missions indicates that the impact fluxes were decreasing during the stages of mare formation. An exponentially decaying flux for the last 3.5 b.y. with a half-life of 0.6 to 1.4 b.y. is compatible with the data.

Soderblom, L. A.↗
NASA NTRS1973

Chemical evolution of cosmic clouds

Reaction rate characteristics of interstellar matter were studied by the reaction of hydrogen cyanide and molecular hydrogen at about 1000 K at an HCN to H2 ratio of 1 to 100 to simulate the large excess of cosmic hydrogen. It was found that HCN decays with a half life of about 20 hours and that a large surface increases the reaction rate as a function of temperature. Reaction rates may be considerable increased by energetic processes that produce free radicals and ions.

Down, B. D.↗
NASA NTRS1972

Search for extinct natural radioactivity of Pb205 via thallium-isotope anomalies in chondrites and lunar soil.

Thallium and Pb204 contents were determined by stable-isotope-dilution analysis in 16 chondrites, one achondrite, and Apollo 11 and 12 lunar fines. Meteoritic thallium contents vary over a large range, 0.02 to 100 ppb, corresponding to the fact that thallium is a highly fractionated volatile element. Lunar thallium contents are less than 5 ppb. The Tl205/Tl203 ratio was determined in most of the samples, with precision ranging from 0.03% to several percent depending mainly on the amount of thallium present. No variations from the terrestrial ratio were observed. The chondritic isochron slope for Pb205 (13.8-m.y. half-life) is less than or equal to 0.00009 (99% confidence level), corresponding to an interval of at least 60 m.y. and possibly exceeding 120 m.y. between the termination of s-process nucleosynthesis and the lead-thallium fractionations.

Huey, J. M.↗
NASA NTRS1973

Alpha particles in solar cosmic rays over the last 80,000 years.

Present-day (1967 to 1969) fluxes of alpha particles from solar cosmic rays, determined from satellite measurements, were used to calculate the production rates of cobalt-57, cobalt-58, and nickel-59 in lunar surface samples. Comparisons with the activities of nickel-59 (half-life, 80,000 years) measured in lunar samples indicate that the long-term and present-day fluxes of solar alpha particles are comparable within a factor of approximately 4.

Lanzerotti, L. J.↗
NASA NTRS1973

Re-187, recycling r-process elements through stars, and the age of the Galaxy.

The enhanced beta-decay rate of ionized Re-187 in stars has been studied within the context of a detailed numerical model of the production of r-process elements and their recycling through stars during the course of galactic evolution. It is concluded that the enhanced decay rate does not significantly reduce the Re-Os chronometer age for the Galaxy. Consequently, the Re-187 beta-decay half-life and the Os-186/Os-187 neutron cross-section ratio remain as the significant uncertainties in this chronology. Unlike the uncertainties in other chronologies, both are amenable to laboratory measurements.

Talbot, R. J., Jr.↗
NASA NTRS1972

The origin and chemical composition of the earth's core

The process of core formation in the earth is subject to the constraints that it be nearly simultaneous with accretion and yet occur in a manner that the mantle retains radiogenic Xe-129 produced from the extinct radioactivity of I-129 with a half life of 17.6 million y. From these constraints, it appears that the only feasible mechanism is the segregation of an Fe-FeS melt. Trace element abundances in major classes of meteorites and the silicate fractions of the earth show that not only there is a high depletion of sulphur in the crust and the mantle, but that it is even more highly depleted than the rare gases, water and the halogens. From the nature of this depletion pattern and the fact that any model of accretion of the earth will necessarily produce an Fe-FeS melt, it is concluded that the light element in the core is largely sulphur with minor amounts of carbon. A consequence of this mode of core formation is found to be the availability of K-40 radioactive heat production in the liquid core, estimated at about 10 to the 19th power erg/s at the present time.

Murthy, V. R.↗
NASA NTRS1974

M558 radioactive tracer diffusion

This experiment was performed in Skylab 3 with two objectives in mind. First, the experimental self-diffusion coefficients for liquid zinc were to be determined in a convection-free environment. Secondly the reduction in convective mixing in earth gravity by going into the zero-gravity environment of space was to be estimated. The experiment was designed to utilize high temperatures and linear thermal gradients provided by the M518 Multipurpose Electric Furnace, and the radioactivity of zinc-65 of 245-day half-life to investigate self-diffusion in liquid zinc. The distribution of zinc-65 tracer, after melting, maintaining at soak temperature for 1 hour of soak time and then resolidifying, was obtained by sample sectioning. The concentration of activity of each section (microcurie-gram) was plotted against positions along the sample axial and radial position. Experimental data and theoretical results from solution of Fick's law of diffusion in one dimensional were compared. Samples tested on earth showed very rapid diffusion. Diffusion coefficient in unit gravity was 50 times the zero-gravity diffusion coefficient of Skylab.

Ukanwa, A. O.↗
NASA NTRS1974

Measurements of the cosmic-ray Be/B ratio and the age of cosmic rays

The ratio Be/B depends on whether the confinement time of cosmic rays in the Galaxy is long or short compared to the radioactive half-life of Be-10. We report observations of this ratio which were obtained with a dE/dx-Cerenkov detector launched into a polar orbit on OGO-6 as part of the Caltech Solar and Galactic Cosmic Ray Experiment. Be/B ratios were determined for various rigidity thresholds up to 15 GV. We find no statistically significant rigidity dependence of the ratio, which is 0.41 plus or minus 0.02 when averaged over all observed cutoffs. Additional calculations suggest that if the present fragmentation parameters are correct, then the lifetime of cosmic rays in the Galaxy is less then 10 m.y.

Brown, J. W.↗
NASA NTRS1974

Meteoritic material on the moon

Micrometeorites, ancient planetesimal debris from the early intense bombardment, and debris of recent, crater-forming projectiles are discussed and their amounts and compositions have been determined from trace element studies. The micrometeorite component is uniformly distrubuted over the entire lunar surface, but is seen most clearly in mare soils whereas, the ancient component is seen in highland breccias and soils. A few properties of the basin-forming objects are inferred from the trace element data. An attempt is made to reconstruct the bombardment history of the moon from the observation that only basin-forming objects fell on the moon after crustal differentiation. The apparent half-life of basin-forming bodies is close to the calculated value for earth-crossing planetesimals. It is shown that a gap in radiometric ages is expected between the Imbrium and Nectaris impacts, because all 7 basins formed in this interval lie on the farside or east limb.

Morgan, J. W.↗