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At least 667 records · Page 37

Characterization of Tank 9H Annulus Sample in Support of Residual Material Inventory Determinations

The Savannah River National Laboratory (SRNL) was requested by Savannah River Mission Completion (SRMC) to provide sample preparation and characterization of the Tank 9H annulus sample in support of Residual Material Inventory Determinations. One Tank 9H sample in three vials [HTF-9-25-13, HTF-9-25-14 and HTF-9-25-15], with each vial containing approximately 200 mL of the Tank 9H annulus salt solution, were delivered to the SRNL Shielded Cells for sample preparation and characterizations in February 2025. The density of the “as-received” solution contained in each of the three Tank 9H annulus sample vials were determined followed by a solid-liquid separation on each one using 0.45-micron Nalgene® nylon filter membranes. The resulting filtrates were combined to form the Tank 9H annulus sample with a total volume of about 600 mL. The combined wet solid fractions, about a total of 4.8 grams of salt material, remaining on the filter membranes were air-dried in the Shielded Cells for 72 hours. The total weight of the air-dried solids was 2.1 grams. These air-dried solids were washed with deionized water (DI water) at a phase ratio of 60 mL DI water/gram of solids to recover insoluble solids, if any. No visible or measurable quantity of insoluble solids were recovered after DI water washing of the air-dried solids because the air-dried solids completely dissolved in the DI water. The solid fraction-wash water was not combined with the 600 mL of the filtrate solution, and the resulting solution was not screened or analyzed for radionuclides. Aliquot sample volumes of the undiluted Tank 9H annulus sample were sent to the SRNL analytical services groups for radionuclides, elementals, anions and total mercury analysis by various methods including radiochemical separations/counting methods, inductively coupled plasma-atomic emission spectroscopy (ICP-AES), and Inductively Coupled Plasma Mass Spectroscopy (ICP-MS) and special preparations. All sample analyses were performed in triplicate. This report presents the analytical characterization results for the Tank 9H annulus sample. The results are also reported where analytical methods yielded additional analytes, other than those requested by SRMC. In the characterization of the Tank 9H annulus sample, the detection limits for all the analytes, as specified in the Technical Task Request (TTR) and Task Technical and Quality Assurance Plan (TTQAP), were met.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

CWMD Nuclear Forensics Quarterly Report

Analysis and evaluation of nuclear debris is a key component to identify forensic signatures in a post-detonation environment. Currently, methods exist and are practiced in obtaining signatures from post-detonation debris. However, efforts to reduce the timeline in obtaining signatures is continuous within nuclear forensics research and will be forwarded by this research. This education and research project will explore combined material chemistry and separations of radionuclides to provide actionable signatures in less time than standard methods. The research will use the phase distribution of radionuclides in debris to develop targeted and rapid dissolution methods. These dissolution methods will be coupled with microfluidics to achieve samples suitable for analysis within reduced timelines.

and nuclear chemistry↗

Integrated Security-Safety Consequence Study of a Heat Pipe Reactor

This report presents a preliminary demonstration of integrated security/safety consequence modeling to support potential physical security exemption justifications under the new Title 10 Code of Federal Regulations Part 53 licensing pathway, which allows exemptions if sabotage-induced radiological consequences do not exceed 25 rem at the site boundary two hours after release without mitigative actions. A hypothetical heat pipe microreactor subjected to direct sabotage by a 150 lbs. TNT-equivalent high-explosive device was analyzed using a simplified radionuclide release estimate based on DOE-HDBK-3010-94, implemented in the MELCOR severe accident analysis code to model release transport and attenuation through reactor/building compartments, with MELCOR outputs coupled to MACCS to compute offsite doses and the distance-to-threshold metric D 25rem . Six scenarios were evaluated to examine sensitivities to release pathway/building configuration and radionuclide form (vapor versus aerosols with different size distributions). Results show a positive correlation between leak path factor and D 25rem and indicate that reactor building compartmentalization can substantially reduce consequences (a single-story configuration reduced D 25rem by roughly an order of magnitude relative to a cavity-only configuration), while vapor versus aerosol assumptions had limited impact for the modeled two-story case on the spatial grid used.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

A computational pipeline to generate a synthetic dataset of metal ion sorption to oxides for AI/ML exploration

The charged mineral/electrolyte interfaces are ubiquitous in the surface and subsurface–including the surroundings of the geological disposal sites for radioactive waste. Therefore, understanding how ions interact with charged surfaces is critically important for predicting radionuclide mobility in the case of waste leakage. At present, the Surface Complexation Models (SCMs) are the most successful thermodynamic frameworks to describe ion retention by mineral surfaces. SCMs are interfacial speciation models that account for the effect of the electric field generated by charged surfaces on sorption equilibria. These models have been successfully used to analyze and interpret a broad range of experimental observations including potentiometric and electrokinetic titrations or spectroscopy. Unfortunately, many of the current procedures to solve and fit SCM to experimental data are not optimal, which leads to a non-transferable or non-unique description of interfacial electrostatics and consequently of the strength and extent of ion retention by mineral surfaces. Recent developments in Artificial Intelligence (AI) offer a new avenue to replace SCM solvers and fitting algorithms with trained AI surrogates. Unfortunately, there is a lack of a standardized dataset covering a wide range of SCM parameter values available for AI exploration and training–a gap filled by this study. Here, we described the computational pipeline to generate synthetic SCM data and discussed approaches to transform this dataset into AI-learnable input. First, we used this pipeline to generate a synthetic dataset of electrostatic properties for a broad range of the prototypical oxide/electrolyte interfaces. The next step is to extend this dataset to include complex radionuclide sorption and complexation, and finally, to provide trained AI architectures able to infer SCMs parameter values rapidly from experimental data. Here, we illustrated the AI-surrogate development using the ensemble learning algorithms, such as Random Forest and Gradient Boosting. These surrogate models allow a rapid prediction of the SCM model parameters, do not rely on an initial guess, and guarantee convergence in all cases.

Li, Chunhui↗

An Alternative Conceptual Model for the Spent Nuclear Fuel–Water Interaction in Deep Geologic Disposal Conditions

For the long-term safety assessment of direct disposal of spent nuclear fuel in deep geologic repositories, knowledge on the radionuclide release rate from the UO 2 matrix is essential. This work provides a conceptual model to explain the results of leaching experiments involving used nuclear fuel or simulant materials in confirmed reducing conditions. Key elements of this model are: direct effect of radiation from radiolytic species (including defects and excited states) in the solid and in the first water layers in contact with its surface; and excess H 2 may be produced due to processes occurring at the surface of the spent fuel and in confined water volumes, which may also play a role in keeping the spent fuel surface in a reduced state. The implication is that the fractional radionuclide release rate used in most long-term safety assessments (10 -7 year -1 ) is over estimated because it assumes that there is net UO 2 oxidation caused by radiolysis, in contrast with the alternative conceptual model presented here. Furthermore, conventional water radiolysis models and radiation chemical yields published in the literature are not directly applicable to a heterogeneous system such as the spent fuel–water interface. Suggestions are provided for future work to develop more reliable models for the long-term safety assessment of spent nuclear fuel disposal.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Uranium (VI) Adsorbate Structures on Portlandite [Ca(OH)2] Type Surfaces Determined by Computational Modelling and X-ray Absorption Spectroscopy

Portlandite [Ca(OH) 2 ] is a potentially dominant solid phase in the high pH fluids expected within the cementitious engineered barriers of Geological Disposal Facilities (GDF). This study combined X-ray Absorption Spectroscopy with computational modelling in order to provide atomic-scale data which improves our understanding of how a critically important radionuclide (U) will be adsorbed onto this phase under conditions relevant to a GDF environment. Such data are fundamental for predicting radionuclide mass transfer. Surface coordination chemistry and speciation of uranium with portlandite [Ca(OH) 2 ] under alkaline groundwater conditions (ca. pH 12) were determined by both in situ and ex situ grazing incidence extended X-ray absorption fine structure analysis (EXAFS) and by computational modelling at the atomic level. Free energies of sorption of aqueous uranyl hydroxides, [UO 2 (OH) n ] 2–n (n = 0–5) with the (001), (100) and (203) or (101) surfaces of portlandite are predicted from the potential of mean force using classical molecular umbrella sampling simulation methods and the structural interactions are further explored using fully periodic density functional theory computations. Although uranyl is predicted to only weakly adsorb to the (001) and (100) clean surfaces, there should be significantly stronger interactions with the (203/101) surface or at hydroxyl vacancies, both prevalent under groundwater conditions. The uranyl surface complex is typically found to include four equatorially coordinated hydroxyl ligands, forming an inner-sphere sorbate by direct interaction of a uranyl oxygen with surface calcium ions in both the (001) and (203/101) cases. In contrast, on the (100) surface, uranyl is sorbed with its axis more parallel to the surface plane. The EXAFS data are largely consistent with a surface structural layer or film similar to calcium uranate, but also show distinct uranyl characteristics, with the uranyl ion exhibiting the classic dioxygenyl oxygens at 1.8 Å and between four and five equatorial oxygen atoms at distances between 2.28 and 2.35 Å from the central U absorber. These experimental data are wholly consistent with the adsorbate configuration predicted by the computational models. These findings suggest that, under the strongly alkaline conditions of a cementitious backfill engineered barrier, there would be significant uptake of uranyl by portlandite to inhibit the mobility of U(VI) from the near field of a geological disposal facility.

36 MATERIALS SCIENCE↗

Titanium-45 (45Ti) Radiochemistry and Applications in Molecular Imaging

Molecular imaging is an important part of modern medicine which enables the non-invasive identification and characterization of diseases. With the advancement of radiochemistry and scanner technology, nuclear medicine is providing insight into efficient treatment options for individual patients. Titanium-45 (45Ti) is a lesser-explored radionuclide that is garnering increasing interest for the development of positron emission tomography (PET) radiopharmaceuticals. This review discusses aspects of this radionuclide including production, purification, radiochemistry development, and molecular imaging studies.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

An Updated Picture of Presolar History from Short-lived Radioactive Isotopes and Inferences on the Birth of the Sun

We examine the origin of the short-lived radionuclides (SLRs; defined as having half-lives between 0.1 and 100 Ma) present in the early solar system (ESS) by investigating how predictions of their abundances in the interstellar medium (ISM) from steady-state equilibrium relate to their ESS values. For this, we take into account the non-negligible time t iso elapsed between the isolation of the presolar molecular cloud and the formation of the ESS, during which the SLRs decayed freely. We also consider the alternative scenario in which the presolar molecular cloud remained partially mixed with the ISM, with a mixing timescale t mix . We find that the ESS abundances of 107 Pd and 182 Hf produced by slow neutron captures (s-process) and of 53 Mn and 60 Fe produced by explosive nucleosynthesis can be consistently explained within these scenarios. Their required tiso is 9–12 Ma and their required tmix is 11–14 Ma (with one potential exception of t mix = 38 Ma), depending on galactic uncertainties, such as the galactic star formation history and efficiency and the star-to-gas mass ratio. Another s -process SLR, 205 Pb, has a more uncertain ESS value and falls within only some of these time values. The same applies to the SLRs produced by the p -process ( 92 Nb and 146 Sm), depending on the latter’s half-life. In agreement with previous studies, we find that the ESS abundances of the rapid neutron-capture isotopes ( 129 I, 244 Pu, and 247 Cm) and of the most short-lived radionuclides ( 26 Al, 36 Cl, and 41 Ca) cannot be explained by assuming steady-state equilibrium in the ISM.

79 ASTRONOMY AND ASTROPHYSICS↗

The Measurement of Radiation Exposure of Astronauts by Radiochemical Techniques

The principal gamma-ray-omitting radioisotopes produced in the body of astronauts by cosmic-ray bombardment which have half-lives long enough to be useful for radiation dose evaluation are Be-7, Na-22, and Na-24. The sodium isotopes were measured in the preflight and postflight urine and feces, and those feces specimens collected during the manned Apollo missions, by analysis of the urine salts and the raw feces in large crystal multidimensional gamma-ray spectrometers. The Be-7 was chemically separated, and its concentration measured in an all Na(T1), anticoincidence shielded, scintillation well crystal. The overall sensitivity of the experiment was reduced by almost all variables such as low concentrations of excreted cosmogenic radionuclides, high concentrations of injected radionuclides, low sample sizes, long delay periods before analysis, and uncertain excretion rates. The astronaut radiation dose in millirads, as determined by this technique, for the Apollo 7, 8, 9, 10, 11, 12, and 13 missions was 330, 160, 315, 870 ? 550, 31, 110, and 250 respectively. In view of these limitations this technique would be best applied to cases of unusually high exposures, such as that encountered from solar flares.

R L Brodzinski↗

Nuclear chemistry of returned lunar samples: Nuclide analysis by gamma-ray spectrometry

Concentrations of primordial radioelements and of cosmogenic radionuclides in crystalline rocks, breccias, and soils from the Ocean of Storms were determined. Concentrations of K, Th, U, Al-26, and Na-22 were determined for seven clastic or brecciated rocks, three sieved samples of fines, and one composite sample of sawdust from the cutting of a fragmental rock, all from samples obtained on the Apollo 14 mission. The K, Th, and U concentrations and cogmogenic radionuclide abundances in rocks and soils from Apollo 15 are also discussed.

Kelley, G. D.↗

Calculation of the lunar photon albedo from galactic and solar proton bombardment.

The lunar photon albedo due to cosmogenic and primordial photon sources has been calculated. The individual photon leakage spectra from prompt photons produced by galactic cosmic ray (GCR) and solar cosmic ray (SCR) induced nuclear interactions, from the decay of GCR- and SCR-induced radionuclides, and from the decay of naturally occurring radionuclides are given. An approximate estimate of the leakage from the photon-electron cascade initiated by the decay of neutral pions is also given. Monte Carlo methods have been used to determine the nucleon-meson cascade, and discrete-ordinates methods were used for the photon and low-energy neutron transport.

Armstrong, T. W.↗

Thermal history and early magmatism in the moon.

Lunar heat-flow calculations are carried out for a model moon in which (1) near-surface initial temperatures are very high (as the occurrence of a surface anorthositic layer seems to require), and (2) heat-generating radionuclides are transported upward when melting occurs. Near-surface regions are found to cool and then experience a resurgence of high temperature, as radionuclide-rich magmas from the lunar interior accumulate near the surface. This peaking of near-surface temperature can be brought into correspondence with the episode of vulcanism that gave rise to the basalts represented in the Apollo samples, if we assume relatively high lunar temperatures in early times (due to high initial temperatures, or a high content of radioactive elements, or both).

Wood, J. A.↗

The degassing history of the Earth: Noble gas studies of Archaean cherts and zero age glassy submarine basalts

Recent noble gas studies suggests the Earth's atmosphere outgassed from the Earth's upper mantle synchronous with sea floor spreading, ocean ridge hydrothermal activity and the formation of continents by partial melting in subduction zones. The evidence for formation of the atmosphere by outgassing of the mantle is the presence of radionuclides H3.-4, Ar-040 and 136 Xe-136 in the atmosphere that were produced from K-40, U and Th in the mantle. How these radionuclides were formed is reviewed.

Hart, R.↗

Cosmic ray records in Antarctic meteorites

The cosmogenic radionuclides Be(10), Al(26), and Mn(53) and noble gases were determined in more than 28 meteorites from Antarctica by nuclear analytical techniques and static mass spectrometry, respectively. The summarized results are listed. The concentrations of Al(26) and Mn(53) are normalized to the repective main target elements and given in dpm/kg Si sub eq and dpm/kg Fe. The errors stated include statistical as well as systematical errors. For noble gas concentrations estimated errors are 5% and for isotopic ratios 1.5%. Cosmic ray exposure ages T sub 21 were calculated by the noble gas concentrations and the terrestrial residence time (T) on the basis of the spallogenic nuclide Al(26). The suggested pairing of the LL6 chondrite RKPA 80238 and RKPA 80248 and the eucrites ALHA 76005 and ALHA 79017 is confirmed not only by the noble gas data but also by the concentrations of the spallation produced radionuclides. Futhermore, ALHA 80122, clasified as an H6 chondrite, has a noble gas pattern which suggest that this meteorite belongs to the ALHA 80111 shower.

Vogt, S.↗

Terrestrial ages of Antarctic meteorites: Implications for concentration mechanisms

Antarctic meteorites differ from meteorites fallen in other places in their mean terrestrial ages. Boeckl estimated the terrestrial half-life for the disintegration of stone meteorites by weathering under the climatic conditions of the Western United States to be about 3600 years. Antarctic meteorites, however, have terrestrial ages up to 70000 years, indicating larger weathering half-lives. The terrestrial ages of meteorites are determined by their concentration of cosmic-ray-produced radionuclides with suitable half-lives (C-14, Al-26, and Cl-36). These radionuclides have yielded reliable ages for the Antarctic meteorites. The distribution of terrestrial ages of Allan Hills and Yamato meteorites are examined.

Schultz, L.↗

Cosmogenic neutron-capture-produced nuclides in stony meteorites

The complete neutron-flux results and production rates for Cl-36, Ni-59, and Co-60 in stony meteorites of various radii and composition are presented. The relative neutron source strengths and neutron production-versus-depth profiles were determined by using calculated H-3 production rates. The absolute source strengths were normalized to that determined for the moon by Woolum et al. (1975). The energy spectrum of the source neutrons and the neutron transport calculations, which employed the ANISN computer code, were similar to those used for the moon by Lingenfelter et al. (1972). The production rates of the three radionuclides were determined as a function of depth in various spherical meteoroids from the calculated equilibrium neutron-flux distributions and from energy-dependent neutron-capture cross sections. Rates for producing these radionuclides by spallation reactions were also calculated.

Spergel, M. S.↗

Evidence of the in situ decay of Al-26 in a Semarkona chondrule

A long-standing problem in the study of meteorites, with broad implications for the evolution of the solar system, is the source of heat for melting small planets. Meteorites, such as the eucrites, were obviously the result of a melting process on a small planet, yet the decay of the long-lived radionuclides present on the earth, K-40, U-235, U-238, and Th-232, could not have provided nearly enough heat to initiate melting approximately 4.5 aeons ago, even on bodies 1000 km in diameter. This problem addressed by H.C. Urey in 1955, who recognized that the presence of short-lived (and now extinct) radionuclides such as Al-26 (half-life of approximately 720,000 y) in the early solar system would have provided an abundant heat source for melting small asteroid-size bodies. Since any Al-26 initially present in the solar nebula would have completely decayed after only a few tens of millions of years, the problem became one of finding evidence of Al-26, in the form of excess Mg-26, in meteorites. The search for evidence of the Al-26 is briefly examined.

Hutcheon, I. D.↗

Radioactivities of Long Duration Exposure Facility (LDEF) materials: Baggage and bonanzas

Radioactivities in materials onboard the returned Long Duration Exposure Facility (LDEF) satellite were studied by a variety of techniques. Among the most powerful is low background Ge semiconductor detector gamma ray spectrometry. The observed radioactivities are of two origins: those radionuclides produced by nuclear reactions with the radiation field in orbit and radionuclides present initially as contaminants in materials used for construction of the spacecraft and experimental assemblies. In the first category are experiment related monitor foils and tomato seeds, and such spacecraft materials as Al, stainless steel, and Ti. In the second category are Al, Be, Ti, Va, and some special glasses. Consider that measured peak-area count rates from both categories range from a high value of about 1 count per minute down to less than 0.001 count per minute. Successful measurement of count rates toward the low end of this range can be achieved only through low background techniques, such as used to obtain the results presented here.

Smith, Alan R.↗