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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Measurement of the 230 Th( p ,2n)Pa229 and 230 Th( p ,3n)Pa228 reaction cross sections from 14.1 to 16.9 MeV

Actinium-225 is of interest for medical isotope production and there is on-going research into methods of producing Ac 225 , either directly or via the decay of its parent isotopes ( Th 229 , Pa 229 , and Ra 225 ). One method that has been suggested is the Th 230 ( p , 2 n ) Pa 229 reaction. However, there is no available cross-section data for this reaction in the literature. Purpose: Measure the Th 230 ( p , 2 n ) and Th 230 ( p , 3 n ) reaction cross sections in the energy range where the ( p , 2 n ) reaction is predicted to peak to determine the feasibility of Ac 225 production via the Th 230 ( p , 2 n ) reaction. Methods: Targets naturally enriched in Th 230 were irradiated at the Center for Accelerator Mass Spectrometry at Lawrence Livermore National Laboratory with energies ranging from 14.1 to 16.9 MeV. Furthermore, chemical processing was used to separate the protactinium activation products, followed by γ -ray spectroscopy to measure the activities of Pa 228 , 229 , 230 , 232 produced in the irradiation. Results: We find that excitation functions are reported for the first time in the literature for the Th 230 ( p , 2 n ) and Th 230 ( p , 3 n ) reactions in this energy range. The peak measured value of the Th 230 ( p , 2 n ) reaction was found to be 182 ± 12 mb at 14.4 ± 0.1 MeV. The Th 232 ( p , n ) Pa 232 reaction was used to verify the experimental conditions, the measured values are reported and are comparable to the existing literature values. From the γ -ray spectrometry data, the half-life of Pa 229 was measured as 1.5 ± 0.1 days, which is within the error of the half-life reported in the evaluated nuclear data as well as in the recent measurements, and the half-life of Pa 228 was measured as 19.5 ± 0.4 hours. Conclusions: Overall, the Th 230 ( p , 2 n ) Pa 229 reaction could reasonably be used for Ac 225 isotope production, although significant amounts of relatively isotopically pure Th 230 would be needed for significant production because the low alpha-decay branching ratio of Pa 229 and long half-life of Th 229 inhibit the in-growth of significant amounts of Ac 225 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Literature Data on Foam Fracturing Fluid

At the beginning of this project, the Temple team spent significant effort to collect data relevant to foam fracturing. More than 40 articles/reports were found in the open literature that reported the properties of aqueous foams under various testing conditions. The foam properties included viscosity and stability in terms of half-life, while were influenced by the foam quality, shear rate, temperature, pressure, as well as surfactants and additives used in making the foam base solutions. As a result, more than 1100 data points were collected, which are included in a master worksheet named "Literature data on Foam Fracturing Fluid". These data points are organized based on following parameters: 1. Literature source, including authors and publication year 2. Gaseous phase (e.g. CO2, N2) 3. Liquid phase (e.g. tap water, DI water, salt water) 4. Surfactants and their concentrations 6. Additives 7. Foam quality 8. Pressure 9. Temperature 10. Viscosity 11. Foam stability, which was characterized by its half-life: Half-life Foam study data base with data analysis was completed and a webpage is designed hosted on public server at https://surfactant-dashboard.herokuapp.com

15 GEOTHERMAL ENERGY↗
DOE OSTI2020

Design Optimization of A generic Fissile Solution for Mo99 production using Electron Beam-based Neutron Generator using MCNP+CFD

Molybdenum-99 ( 99 Mo) is a medical isotope used in 80% of all medical imaging procedures today. However, 99 Mo is not directly administered to patients for imaging; its decay product, technetium-99m ( 99 mTc), is a metastable isotope with a half-life of ~6 hours. Such a short half-life does not allow for production, separation, and application to a patient before decaying further. Therefore, the solution is to produce the precursor to 99 mTc, 99 Mo. 99 Mo has a half-life of 66 hours, long enough to produce the material and send it to the desired location before it fully decays. Under National Nuclear Security Administration’s (NNSA) highly enriched uranium (HEU) minimization mission, the Material Management and Minimization (M3) office leads the Molybdenum-99 (Mo-99) program. A major goal of the Mo-99 program is to develop methods of producing 99 Mo using low enriched uranium (LEU) opposed to the traditionally used HEU domestically in the U.S. Internationally, LEU is the new standard for use in research reactors and isotope production facility. In this study, we introduce a generic fissile solution system for 99 Mo production facility meeting the design requirement of 1) LEU usage as fissile material and 2) subcritical fissile system coupled with a horizontal electron beam (E-beam) accelerator. The focus of this research is to optimize a fissile solution configuration for maximum 99 Mo production yield using MCNP model, and ultimately implement the optimized design with computational fluid dynamics (CFD) model to understand thermal hydraulic behavior and solution convection characteristic. The report consists of two parts: 1) isotope yield calculation and criticality analysis with a wide range of parametric test matrix, and 2) thermal hydraulic analysis for solution mixing and cooling assessment.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2022

New results from the CUORE experiment

We report that the Cryogenic Underground Observatory for Rare Events (CUORE) is the first bolometric experiment searching for neutrino-less double-beta (0vββ) decay that has been able to reach the one-ton scale. The detector, located at the Laboratori Nazionali del Gran Sasso in Italy, consists of an array of 988 TeO 2 crystals arranged in a compact cylindrical structure of 19 towers. Following the completion of the detector construction in August 2016, CUORE began its first physics data run in 2017 at a base temperature of about 10 mK. Following multiple optimization campaigns in 2018, CUORE is currently in stable operating mode. In 2019, CUORE released its second result of the search for 0vββ corresponding to a TeO 2 exposure of 372.5 kg∙yr and a median exclusion sensitivity to a 130 Te 0vββ decay half-life of 1.7 ∙ 10 25 yr. We find no evidence for 0vββ decay and set a 90% C.I. Bayesian lower limit of 3.2 ∙ 10 25 yr on the 130 Te 0vββ decay half-life. We present the current status of CUORE’s search for 0vββ. We give an update of the CUORE background model and the measurement of the 130 Te two neutrino double-beta (2vββ) decay half-life. Eventually, we show the preliminary results on half-life limits from the analysis of 130 Te 0vββ and 2vββ decay to the first 0 + excited state of 130 Xe.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

In vivo pharmacokinetic enhancement of monomeric Fc and monovalent bispecific designs through structural guidance

In a biologic therapeutic landscape that requires versatility in targeting specificity, valency and half-life modulation, the monomeric Fc fusion platform holds exciting potential for the creation of a class of monovalent protein therapeutics that includes fusion proteins and bispecific targeting molecules. Here we report a structure-guided approach to engineer monomeric Fc molecules to adapt multiple versions of half-life extension modifications. Co-crystal structures of these monomeric Fc variants with Fc neonatal receptor (FcRn) shed light into the binding interactions that could serve as a guide for engineering the half-life of antibody Fc fragments. These engineered monomeric Fc molecules also enabled the generation of a novel monovalent bispecific molecular design, which translated the FcRn binding enhancement to improvement of in vivo serum half-life.

59 BASIC BIOLOGICAL SCIENCES↗
NASA NTRS1973

Solar flare proton spectrum averaged over the last 5000 years

The solar flare differential energy spectrum and integral proton flux above 10 MeV averaged over the last several thousand years are derived from thermoluminescence (TL) data. The dose-rate depth profile is obtained using a new TL equilibrium technique which is independent of the TL decay kinetics. The dose-rate depth profile produced by solar flare protons with a differential energy spectrum of the form dJ/dE = KE to the minus gamma power is calculated for arbitrary gamma. The best fit to the TL data in rock 14310 is obtained for gamma = 2.3 plus or minus 0.2 and an omnidirectional (4 pi) integral flux above 10 MeV of 40 to 80 prot/sq cm/sec. The TL half-life is determined to be 2000 yr. These results are compared to those for Na-22 (half-life of. 2.6 yr) and Al-26 (half-life of 740,000 yr) obtained by Wahlen et al. (1972) and Rancitelli et al. (1972), and it is concluded that the spectral shape and flux of protons in the interval from 25 to 100 MeV is the same within experimental errors when averaged over these three very different time periods.

Hoyt, H. P., Jr.↗
NASA NTRS1983

Hf chronometer for the early solar system

It is now widely believed that Al-26 (half-life, 7.2 x 10 to the 5th yr) and Pd-107 (half-life, 6.5 x 10 to the 6th yr) were present in the early solar system. The nucleosynthetic event responsible for the production of these nuclei must therefore have occurred no more than a few million years before the formation of solid bodies. It is possible that this event also gave a rise to the I-129 believed to be present in the early solar system. The last event to contribute Pu-244 to the solar system, however, occurred approximately 10 to the 8th yr before the time of solidification. It is noted that this latter time scale is also consistent with the lack of evidence for a Cm-247 chronometer. It is proposed that Hf-182 (half-life, 9 x 10 to the 6th yr) can resolve the question whether heavy-element nonactinide nucleosynthesis occurred during the (Al-26)-producing event. It is believed that an answer to this question will help to clarify the chronology of the formation of the solar system and will help to determine the astrophysical sites of heavy-element nucleosynthesis.

Norman, E. B.↗
DOE OSTI2025

Hydrogen influences thermal activation parameters for dislocation glide during low cycle fatigue of 316L stainless steel

Measurements of activation areas are used to investigate the effect of hydrogen on the kinetics of dislocation glide during cyclic deformation in cold-worked 316L stainless steel. Non-charged and hydrogen-precharged (H-precharged) specimens were tested in low cycle fatigue (LCF) under plastic strain control. A series of plastic strain rate changes was performed periodically at the peak true plastic strain from the first cycle to half-life, and at various plastic strain values around stable hysteresis loops near half-life to determine the operational activation area, Δ a ∗. Both material conditions demonstrate a rapid increase in Δ a ∗ during the initial rapid softening followed by a region of approximately constant values coinciding with a reduced rate of softening. Near half-life, hydrogen reduces Δ a ∗ at a given true stress due to its effect on the activation distance and obstacle spacing. The magnitudes of Δ a ∗ reveal that bypassing solutes, cutting forest dislocations, and initiating cross slip are important mechanisms of thermally activated dislocation glide at all amplitudes, except hydrogen suppresses cross slip at the lowest plastic strain amplitudes. These results are supported by electron microscopy characterization of deformed microstructures. A Haasen plot analysis indicates that forest dislocations control the kinetics of deformation in both material conditions. It also reveals the presence of athermal obstacles in both non-charged and H-precharged conditions, likely dense dislocation tangles and cell walls. Additionally, the effect of hydrogen on microstructure evolution (by reducing the propensity for cross slip) leads to a dependence of athermal stress on plastic strain amplitude.

Activation area↗
NASA NTRS1994

Measurement of the decay rate of the SiH feature as a function of temperature

We have previously suggested that the SiH fundamental stretch could serve as a diagnostic indicator of the oxidation state of silicate surfaces exposed to the solar wind for prolonged periods. We have now measured the primary decay rate of SiH in vacuo as a function of temperature and find that the primary rate constant for the decay can be characterized by the following equation: k(min(exp -1)) approximately equals 0.186 exp(-9/RT) min(exp -1), where R = 2 x 10(exp -3) kcal deg(exp -1) mole(exp -1). This means that the half-life for the decay of the SiH feature at room temperature is approximately 20 yrs, whereas the half-life at a peak lunar regolith temperature of approximately 500K would be only approximately 20 days. At the somewhat lower temperature of approximately 400K the half-life for the decay is on the order of 200 days. The rate of loss of SiH as a function of temperature provides an upper limit to the quantity of H implanted by the solar wind which can be retained by a silicate grain in a planetary regolith. This will be discussed in more detail here.

Nuth, Joseph A., III↗
NASA NTRS2003

Kinetics of Organic Transformations Under Mild Aqueous Conditions: Implications for the Origin of Life and Its Metabolism

The rates of thermal transformation of organic molecules containing carbon, hydrogen, and oxygen were systematically examined in order to identify the kinetic constraints that governed origin-of-life organic chemistry under mild aqueous conditions. Arrhenius plots of the kinetic data were used to estimate the reaction half-life at 50 C, and to reveal the effect of functional groups on reactivity. This survey showed that hydrocarbons and organic substances containing a single oxygenated group were kinetically the most stable (i. e. acetate decarboxylation half-life was l0(exp 18) years at 50 C); whereas, organic substances containing two oxygenated groups in which one group was a beta-positioned carbonyl group were the most reactive (i. e. acetoacetate decarboxylation half-life was l0(exp-2) years at 50 C). Of all functional groups the beta-positioned carbonyl group (aldehyde or ketone) was the strongest activating group, giving rates of reaction that were up to 10(exp 24)-times faster than rates of similar molecules lacking the beta-carbonyl group. From this knowledge of organic reactivity and the inherent constraints of autocatalytic processes, we concluded that an origins-of-life process based on autocatalytic transformation of C,H,O-substrates was constrained to using the most reactive organic molecules that contain alpha- or beta-carbonyl groups, since small autocatalytic domains of plausible catalytic power that used less reactive substrates could not carry out chemical transformations fast enough to prevent catastrophic efflux (escape) of reaction intermediates. Knowledge of the kinetics of organic transformations is useful, not only in constraining the chemistry of the earliest autocatalytic process related to the origin of life, but also in establishing the relative reactivity of organic molecules on the early Earth and other planets that may or may not be related to the origin of life.

Weber, Arthur L.↗
DOE OSTI2020

A reverse 230 U/ 226 Th radionuclide generator for targeted alpha therapy applications

Thorium-226 (half-life 30.6 m) is a radionuclide of interest for use in targeted alpha therapy applications. Additionally, due to its short half-life, 226 Th must be provided through a radionuclide generator system from its parent 230 U (20.8 d). Furthermore, as the half-life of 226 Th is very short, it should be provided in a form that is directly amenable to use in biomedical applications.

226-Th↗
DOE OSTI2022

Unsymmetric Pentacene- and Pentacenequinone-Fused Porphyrins: Understanding the Effect of Cross- and Linear-Conjugation

Unsymmetric pentacenequinone-fused (cross-conjugated) and pentacene-fused (linear-conjugated) porphyrins were designed and synthesized. The cross-conjugated (AM 1 –AM 3 ) and linear-conjugated (AM 5 –AM 7 ) porphyrins displayed strikingly different sets of optical and electronic properties, both of which are unusual and nontypical of porphyrins. MCD, DFT, and TDDFT calculations suggest that multiple charge transfer states exist in both π-conjugated systems, which contributes to the complex absorption and MCD spectra of these molecular systems. The general Gouterman’s four-orbital model used to explain porphyrin spectroscopy led to contradicting theoretical and experimental data, and is thus not applicable for these molecular systems. The “2 + 4” and “3 + 3” active spaces have been deduced and have proven effective to interpret the absorption and MCD spectra of the pentacenequinone-fused (cross-conjugated) and pentacene-fused (linear-conjugated) porphyrins, respectively. Spectroelectrochemistry of AM 5 –AM 7 revealed broad and intense IR absorptions in the range of 1500–2500 nm, illustrating the exceptional ability of these pentacene-fused systems to accommodate positive charges. A pronounced metal effect was observed for pentacene-fused porphyrins. While pentacene-fused Ni(II) porphyrin (AM 6 ) demonstrated an abnormal ability to stabilize pentacene with a half-life of >28.3 days, the half-life of the free base and Zn(II) counterparts were normal, similar to those of pentacene analogues. This work provides important and useful information on guiding new material designs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2006

Alpha-Voltaic Sources Using Liquid Ga as Conversion Medium

A family of proposed miniature sources of power would exploit the direct conversion of the kinetic energy of alpha particles into electricity. In addition to having long operational lives, these sources are expected to operate with energy-conversion efficiencies from 70 to 90 percent. A power source as proposed (see figure) would be an electrolytic cell in which liquid gallium would serve as both an electrolyte and an energy-conversion medium. The cell would contain an iridium cathode and a zirconium anode. The alpha particles, each with a kinetic energy approx.5.8 MeV, would be emitted by radioactive decay of Cm-244, which has a half-life of 18 years. The Cm-244 source would be positioned so that the a particles would enter the liquid gallium, where their kinetic energy would be dissipated mostly through ionization of Ga atoms, creating Ga(+) ions and free electrons. The electrons would be collected by iridium cathode, and the Ga(+) ions would be neutralized at the zirconium cathode by electrons returning after flowing through an external circuit. Gallium is a candidate for use as the electrolyte and the energy-conversion medium because in the liquid state it is a semimetal: its electrical conductivity is greater than that of a typical semiconductor but small in comparison with the conductivities of metals. Consequently, in liquid gallium, electrons and Ga(+) can exist without immediate recombination and can be moved by electric fields. It is expected that electric fields, resulting at least partly from the difference between the work functions of the electrode metals, would move the electrons and ions to their respective electrodes. The open-circuit potential of the cell is expected to be 1.62 V - equal to the difference between the work functions of iridium and zirconium. Unlike in a solid-state energy conversion medium, the impingement of energetic a particles would not give rise to displacement damage in the liquid gallium. Hence, the cell should have a long life, limited only by the half-life of Cm-244. A cell having a volume less than 25 cu mm, containing 1 curie of Cm-244 (the curie is a unit of radioactivity equal to 3.7 10(exp 10) disintegrations per second) is expected to deliver a current between 7 and 12 mA, which, at the expected open-circuit potential, would provide a power in the approximate range of 11 to 20 mW.

Patel, Jagdish U.↗
NASA NTRS2000

Cosmogenic Radionuclides in Hot Desert Chondrites With Low C-14 Activities

Terrestrial ages of meteorites from hot deserts provide an important tool to estimate meteorite fluxes to the Earth. Most desert meteorites have terrestrial ages less than 40 ky, but a few achondrites from the Sahara region were recently shown to have significantly higher ages, up to approx.100 ky. In general, C-14 (half-life = 5730 y) is the most suited radionuclide to determine terrestrial ages for desert meteorites. However for meteorites with ages >35 ky, the concentration of cosmogenic C-14 has decreased to a level at which it becomes difficult to distinguish between cosmogenic C-14 and terrestrial contamination. These meteorites may therefore be much older than 35 ky. We selected chondrites with low C-14 activities (less than or equal to 2 dpm/kg) for measurements of the concentrations of cosmogenic Cl-36 (half-life= 3.01 x 10(exp 5) y) and Ca-41 (half-life= 1.04 x 10(exp 5) y) in the metal phase. Since the ratio of Ca-41/Cl-36 in the metal phase of chondrites is relatively constant and well known, the measured ratio is a direct measure of the terrestrial age]. A major problem is that most or sometimes all. of the metal in these old "hot desert" meteorites has been oxidized to hydrated Fe-Ni-oxides. Therefore, we also measured the concentrations of Be-10, Al-26 and Cl-36 in the stony phase in order to constrain the terrestrial age as much as possible.

Welten, K. C.↗
NASA NTRS1999

Cosmogenic Radionuclides in Hot Desert Chondrites with Low C-14 Activities: A Progress Report

Terrestrial ages of meteorites from hot deserts provide an important tool to estimate meteorite fluxes to the Earth. Most desert meteorites have terrestrial ages less than 40 ky, but a few achondrites from the Sahara region were recently shown to have significantly higher ages, up to approx. 100 ky. In general, C-14 (half-life = 5730 y) is the most suited radionuclide to determine terrestrial ages for desert meteorites. However for meteorites with ages greater than 35 ky, the concentration of cosmogenic C-14 has decreased to a level at which it becomes difficult to distinguish between cosmogenic C-14 and terrestrial contamination. These meteorites may therefore be much older than 35 ky. We selected chondrites with low C-14 activities (less than or equal to 2 dpm/kg) for measurements of the concentrations of cosmogenic Cl-36 (half-life= 3.01 x 10 (exp 5) y) and Ca-41 (half-life= 1.04 x 10 (exp 5) y) in the metal phase. Since the ratio of Ca-14/Cl-36 in the metal phase of chondrites is relatively constant and well known, the measured ratio is a direct measure of the terrestrial age. A major problem is that most or sometimes all of the metal in these old "hot desert" meteorites has been oxidized to hydrated Fe-Ni-oxides. Therefore, we also measured the concentrations of Be-10, Al-26 and Cl-36 in the stony phase in order to constrain the terrestrial age as much as possible.

Welten, Kees↗
NASA NTRS2003

Endemic Ru Isotopic Anomalies in Iron Meteorites and in Allende

Small variations for Mo isotopes have been observed recently in the Allende meteorite and in iron meteorites, mesosiderites, and pallasites, using ICPMS. Large effects for Mo have been reported for leaches of Orgueil and in SiC and graphite from Murchison. Variations for Mo in bulk Allende and in Murchison have also been presented by NTIMS. Effects in Ru isotopes can define further the preserved exotic r, s, and p contributions in this mass region, and possible effects in Ru-98 and Ru-99 from Tc-98 (4.2 Ma half-life) and Tc-99 (0.21 Ma half-life). Previous attempts at determination of Ru isotopes yielded no resolved effects. The present work represents a substantial improvement in precision over the earlier work. Chemical and mass spectrometric analytical techniques are presented to determine the Ru isotope compositions in terrestrial standards and in meteorites.

Chen, J. H.↗
NASA NTRS2015

Xenon Fractionation and Archean Hydrogen Escape

Xenon is the heaviest gas found in significant quantities in natural planetary atmospheres. It would seem the least likely to escape. Yet there is more evidence for xenon escape from Earth than for any element other than helium and perhaps neon. The most straightforward evidence is that most of the radiogenic Xe from the decay of (129)I (half-life 15.7 Myr) and (244)Pu (half-life 81 Myr) that is Earth's birthright is missing. The missing xenon is often attributed to the impact erosion of early atmospheres of Earth and its ancestors. It is obvious that if most of the radiogenic xenon were driven off by impacts, most of the rest of the atmophiles fared the same fate. The other line of evidence is in the nonradiogenic isotopes of xenon and its silent partner, krypton. Atmospheric xenon is strongly mass fractionated (at about 4% per amu) compared to any known solar system source (Figure 1). This is in stark contrast to krypton, which may not be fractionated at all: atmospheric Kr is slightly heavier than solar Kr (at about 0.5% per amu), but it is the same as in carbonaceous chondrites. Nonradiogenic xenon is also under abundant relative to krypton (the so-called "missing xenon" problem). Together these observations imply that xenon has been subject to fractionating escape and krypton not.

magnetic fields↗
DOE OSTI2022

Engineered human antibodies for the opsonization and killing of Staphylococcus aureus

Gram-positive organisms with their thick envelope cannot be lysed by complement alone. Nonetheless, antibody-binding on the surface can recruit complement and mark these invaders for uptake and killing by phagocytes, a process known as opsonophagocytosis. The crystallizable fragment of immunoglobulins (Fcγ) is key for complement recruitment. The cell surface of S. aureus is coated with Staphylococcal protein A (SpA). SpA captures the Fcγ domain of IgG and interferes with opsonization by anti-S. aureus antibodies. In principle, the Fcγ domain of therapeutic antibodies could be engineered to avoid the inhibitory activity of SpA. However, the SpA-binding site on Fcγ overlaps with that of the neonatal Fc receptor (FcRn), an interaction that is critical for prolonging the half-life of serum IgG. This evolutionary adaptation poses a challenge for the exploration of Fcγ mutants that can both weaken SpA–IgG interactions and retain stability. Here, we use both wild-type and transgenic human FcRn mice to identify antibodies with enhanced half-life and increased opsonophagocytic killing in models of S. aureus infection and demonstrate that antibody-based immunotherapy can be improved by modifying Fcγ. Our experiments also show that by competing for FcRn-binding, staphylococci effectively reduce the half-life of antibodies during infection. These observations may have profound impact in treating cancer, autoimmune, and asthma patients colonized or infected with S. aureus and undergoing monoclonal antibody treatment.

59 BASIC BIOLOGICAL SCIENCES↗