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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Nuclear Data Sheets for A=38☆

All available experimental data of nuclear structure and decay are evaluated for the known nuclides of mass 38 (Mg, Al, Si, P, S, Cl, Ar, K, Ca, Sc, Ti). Detailed results of this evaluation are presented with the best values recommended for level energies, half-lives, γ-ray energies and intensities, decay properties (energies, intensities and placement of radiations), and other spectroscopic information. The {sup 38}Ar nuclide remains as the most extensively studied via various reactions and decays; no excited states are known in {sup 38}Al except for that an isomeric state is tentatively proposed from a recent β-decay measurement (2015St14); the {sup 38}Sc and {sup 38}Ti nuclides remain unidentified, with no experimental references reported for {sup 38}Sc and with a measurement of fragmentation cross sections reported for {sup 38}Ti but finding no evidence of its presence (1996Bl21). This work supersedes the earlier full evaluation of A=38 by J.A. Cameron and B. Singh (2008Ca01).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1979

Sulfur and halogen chemistry of the stratosphere and of volcanic eruption plumes

The major eruption of Volcan de Fuego caused an enhancement of 1.6 x 10 to the 9 kg of SO4(-) in the stratosphere 6 months after the eruption. Measurable changes in nitric acid vapor and particulate chloride were not observed. Subsequent data suggests that HCl was not injected into the stratosphere. The first simultaneous measurement of halogen and sulfur content of gases and particles in explosive eruption plumes is reported. The average percents of elements in particles were sulfur, 2.5 + or - 2.1; chlorine, 18 + or - 12; and fluorine, 38 + or - 29. The average molecular ratio of HCl/SO2 and HCl/HF were 0.41 + or - 0.26 and 14 + or - 12 in the Guatemalan eruption plumes.

Lazrus, A. L.↗
DOE OSTI2021

Electrochemical deposition of amorphous aluminum oxides on lead pipes to prevent lead leaching into the drinking water

Over 5000 public drinking water systems in the US are out of compliance with the Lead and Copper Rule. Lead leaching from lead pipes is limited by the solubility of a naturally occurring scale. Changes in water quality may cause this scale to become more soluble, releasing lead into the drinking water. We propose a novel electrochemical method to prevent lead leaching from lead pipes. In this method, an aluminum wire and an alkaline phosphate electrolyte are inserted into the pipes. The pipes are then anodized for 2 h by using an external power supply, resulting in the electrodeposition of an insoluble aluminum oxide layer on top of the preexisting scale. This technology was tested on lead pipes from the EBMUD water distribution systems located in Berkeley, CA, using recirculating synthetic and actual tap water for 120 days. The untreated pipes leached an average of 23 ppb and 38 ppb of lead respectively, when using free chlorine and monochloramine as disinfection residuals. In contrast, the treated pipes leached 3 ppb and 5 ppb respectively. These results suggest that the proposed treatment has the potential to prevent lead leaching regardless of the disinfection residual and thus should be further explored in a field trial.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Extension of the Plutonium Oxide Nanocluster Family to Include {Pu 16 } and {Pu 22 }

Plutonium(IV) oxide nanoclusters represent an interesting scientific problem regarding structure-function relationships and are also relevant to global concerns surrounding plutonium reprocessing, the remediation of plutonium-contaminated soils, and the storage or disposal of plutonium-containing wastes. Here we report the synthesis of five unique Pu IV oxide nanoclusters containing 38,22, or 16 metal centers and capped only with inorganic ligands, such as chlorine and water, which prevent formation of the extended PuO 2 structure. The products are interrogated through single-crystal X-ray diffraction, bond valence calculations, and comparisons to other known metal-oxide nanoclusters. Of particular interest is the in-corporation of hydroxide linkages into the smaller plutonium oxide nanoclusters, which underscores previous observations and hypotheses regarding the formation of plutonium polymers and colloids.

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

Radiation-induced reaction kinetics of Zn 2+ with e S - and Cl 2 ˙ - in Molten LiCl–KCl eutectic at 400–600 °C

We report molten chloride salts are currently under consideration as combined coolant and liquid fuel for next-generation molten salt nuclear reactors. Unlike complementary light-water reactor technologies, the radiation science underpinning molten salts is in its infancy, and thus requires a fundamental mechanistic investigation to elucidate the radiation-driven chemistry within molten salt reactors. Here we present an electron pulse radiolysis kinetics study into the behaviour of the primary radiolytic species generated in molten chloride systems, i.e., the solvated electron (e S - ) and di-chlorine radical anion (Cl 2 ˙- ). We examine the reaction of e S - with Zn 2+ from 400–600 °C (E a = 30.31 ± 0.09 kJ mol -1 ), and the kinetics and decay mechanisms of Cl 2 ˙- in molten lithium chloride-potassium chloride (LiCl–KCl) eutectic. In the absence of Zn 2+ , the lifetime of e S - was found to be dictated by residual impurities in ostensibly “pure” salts, and thus the observed decay is dependent on sample history rather than being an intrinsic property of the salt. The decay of Cl 2 ˙- is complex, owing to the competition of Cl 2 ˙- disproportionation with several other chemical pathways, one of which involves reduction by radiolytically-produced Zn + species. Overall, the reported findings demonstrate the richness and complexity of chemistry involving the interactions of ionizing radiation with molten salts.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2017

Removal of Tritium from the Gaseous Effluents Produced by the Recovery of Zirconium from Used Fuel Cladding

U.S. regulations will require the removal of tritium ({sup 3}H) from gaseous effluents associated with nuclear fuel reprocessing and recycling. One process that may generate {sup 3}H-containing gaseous effluents is the recovery of zirconium from used fuel cladding. A chlorination process developed by Collins et al. is designed to convert the zirconium present in Zircaloy{sup R} cladding to recoverable ZrCl{sub 4}. The greatest economic benefit from including zirconium recycle as part of a larger used nuclear fuel (UNF) recycle effort would be a decrease in the disposal cost of used fuel cladding. Used fuel cladding is considered high-level waste (HLW). As zirconium is the second largest element by mass (25%) contained in most UNF assemblies (with uranium being the largest), recovery of the zirconium could result in a substantial decrease in the amount of HLW intended for geologic disposition. The reclaimed ZrCl{sub 4} product, if sufficiently free from radioactive impurities, could then be disposed of as low-level waste or reused in nuclear applications. The chlorination process uses chlorine gas (Cl{sub 2}) and an inert carrier such as argon (Ar) to convert the zirconium present in cladding to ZrCl{sub 4}. ZrCl{sub 4} is more volatile than other components in the cladding, causing evaporation of a relatively pure gaseous ZrCl{sub 4} stream. The product ZrCl{sub 4} is recovered as a solid salt by condensation when cooled to less than about 300 deg. C. A fraction of the {sup 3}H (0-96%) produced in nuclear fuel during irradiation is found in zirconium-based cladding, possibly as zirconium hydride (the wide range is a remnant of various researchers' analyses of cladding of various irradiations and cooling times). Heating the cladding to high temperatures, such as would be done during the chlorination process, will release the {sup 3}H. At the temperatures of the zirconium recycle process, the {sup 3}H is likely to react with excess Cl{sub 2} to produce tritiated HCl ({sup 3}HCl), although this could be avoided if the cladding and fuel were treated to remove {sup 3}H prior to chlorination. A previous analysis showed that the concentration of {sup 3}HCl in the off-gas of the zirconium recycle process will be in the range of parts per billion to a few parts per million. Should {sup 3}H mitigation be required for the zirconium recycle process, it will be completed through the abatement of {sup 3}HCl from this off-gas stream. The intent of the testing described in this summary was to conduct proof-of-principle demonstrations for two {sup 3}HCl removal methods. The zirconium recycle off-gas stream differs from many industrial HCl-containing streams in that the concentration of HCl requiring removal is extremely low. Demonstrations of HCl removal at ppm concentrations were not found in the literature, making the proof-of-principle approach attractive as a way to identify the most promising method for continued development. An important consideration throughout these experiments was that current research efforts on the zirconium recycle process are conducted in a hot cell and any {sup 3}HCl removal methods should be easily deployed in a hot-cell environment.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS1999

The Budget and Partitioning of Stratospheric Chlorine During the 1997 Arctic Summer

Volume mixing ratio profiles of HCl, HOCl, ClNO3, CH3Cl, CFC-12, CFC-11, CCl4, HCFC-22, and CFC-113 were measured simultaneously from 9 to 38 km by the Jet Propulsion Laboratory MkIV Fourier Transform Infrared solar absorption spectrometer during two balloon flights from Fairbanks, Alaska (64.8 N), on May 8 and July 8, 1997. The altitude variation of total organic chlorine (CCly) total inorganic chlorine (Cly), and the nearly constant value (3.7 +/- 0.2 ppbv) of their sum (Cl(sub TOT)) demonstrates that the stratospheric chlorine species available to react with O3 are supplied by the decomposition of organic chlorinated compounds whose abundances are well quantified. Measured profiles of HCl and ClNO3 agree well with profiles found by photochemical model (differences < 10% for altitudes below 35 km) constrained by various other constituents measured by MkIV. The production of HCl by ClO + OH plays a relatively small role in the partitioning of HCl and ClNO3 for the sampled air masses. However, better agreement with the measured profiles of HCl and ClNO3 is obtained when this source of HCl is included in the model. Both the measured and calculated [ClNO3]/[HCl] ratios exhibit the expected near linear variation with [O3]2/[CH4] over a broad range of altitudes. MkIV measurements of HCl, ClNO3, and CC1y agree well with ER-2 in situ observations of these quantities for directly comparable air masses. These results demonstrate good understanding of the budget of stratospheric chlorine and that the partitioning of inorganic chlorine is accurately described by photochemical models that employ JPL97 reaction rates and production of HCl from ClO + OH for the environmental conditions encountered: relatively warm temperatures, long periods of solar illumination, and relatively low aerosol surface areas.

Sen, B.↗
NASA NTRS1999

The Budget and Partitioning of Stratospheric Chlorine During the 1997 Arctic Summer

Volume mixing ratio profiles of HCl, HOCl, ClNO3, CH3Cl, CFC-12, and CFC-11, CCl4, HCFC-22, and CFC-113 were measured simultaneously from 9 to 38 km by the Jet Propulsion Laboratory MkIV Fourier Transform Infrared solar absorption spectrometer during two balloon flights from Fairbanks, Alaska (64.8 N), on May 8 and July 8, 1997. The altitude variation of total organic chlorine (CCl(sub y)), total inorganic chlorine (Cl(sub y)), and the nearly constant value (3.7 +/- 0.2 ppbv) of their sum (Cl(sub TOT)) demonstrates that the stratospheric chlorine species available to react with O3 are supplied by the decomposition of organic chlorinated compounds whose abundances are well quantified. Measured profiles of HCl and ClNO3 agree well with profiles found by photochemical model (differences < 10% for altitudes below 35 km) constrained by various other constituents measured by MkIV. The production of HCl by ClO + OH plays a relatively small role in the partitioning of HCl and ClNO3 for the sampled air masses. However, better agreement with the measured profiles of HCl and ClNO3 is obtained when this source of HCl is included in the model. Both the measured and calculated [ClNO3]/[HCl] ratios exhibit the expected near linear variation with [O3](sup 2)/[CH4] over a broad range of altitudes. MkIV measurements of HCl, ClNO3, and CCl(sub y) agree well with ER-2 in situ observations of these quantities for directly comparable air masses. These results demonstrate good understanding of the budget of stratospheric chlorine and that the partitioning of inorganic chlorine is accurately described by photochemical models that employ JPL97 reaction rates and production of HCl from ClO + OH for the environmental conditions encountered: relatively warm temperatures, long periods of solar illumination, and relatively low aerosol surface areas.

Sen, B.↗
DOE OSTI2025

Radiation Effects on the Performance of Advanced Sulfur Monochloride Chlorination Processes

Advanced sulfur chloride-based chlorination technologies are being developed to enable efficient recycling of aluminum and zirconium-based materials used in the nuclear industry. However, the impacts of ionizing radiation on the performance of these sulfur chloride compounds are not well established, despite this being critical knowledge for assessing their feasibility and longevity under envisioned process conditions. Here, in the present article, we report on the effects of cobalt-60 gamma irradiation (≤ 5 MGy) on the aluminum alloy 6061 (AA6061-T6) chlorination yield in sulfur monochloride (S 2 Cl 2 ). Our findings indicate that, compared to nonirradiated solvent, radiation-induced changes in the chemical composition of S 2 Cl 2 —identified using Raman spectroscopy—afford an additional, dose-dependent exothermic process prior to the chlorination reaction’s typical thermodynamic behavior. We attribute this new process to reactions involving aluminum species (metal, oxide, or [oxy]hydroxides) and sulfur dichloride (SCl 2 ), an S 2 Cl 2 radiolysis product that accumulates with absorbed gamma dose, but is absent following an AA6061-T6 chlorination study. Despite the exothermicity of this new process, the overall yield of chlorination decreased with increasing preirradiation dose. Consequently, the chemical reactivity, specificity (aluminum metal vs aluminum passivation and corrosion layer constituents), and byproducts of SCl 2 must be more thoroughly evaluated to support the continued development of advanced S 2 Cl 2 chlorination technologies.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2026

Radiation Effects in Next Generation Used Nuclear Fuel Reprocessing Strategies

With the global community committed to significantly expanding nuclear energy capacity, the development of efficient used nuclear fuel (UNF) management strategies has become more critical than ever. These strategies are vital to fostering the widespread adoption of closed fuel cycles, which are essential for sustainable nuclear energy production and security. Achieving this ambitious goal necessitates a comprehensive understanding of radiation effects on next-generation technologies, as radiolysis can often limit the longevity and performance of these systems. This seminar will provide an overview of next-generation UNF reprocessing strategies, highlighting the latest advancements and innovative approaches in the field. Particular attention will be given to two key areas of recent research: 1. Radiation robustness and performance of advanced sulfur chloride-based chlorination technologies. We will explore the efficacy of sulfur chloride-based chlorination processes in the presence of surrogate cladding materials, specifically aluminum. These processes have shown promise in the dissolution, decontamination, and recovery of cladding materials for reuse. Detailed findings on how the composition and performance of these sulfur chloride solvents respond to radiation exposure will be discussed. 2. Impacts of metal ion complexation and direct dissolution conditions on monoamide-based reprocessing strategies. We will delve into the time-resolved and dose accumulation effects of irradiation on the direct dissolution of voloxidized uranium and rhenium using N,N-di-(2-ethylhexyl) butyramide (DEHBA) or N,N-di-(2-ethylhexyl)isobutyramide (DEHiBA) in pre-equilibrated n-dodecane solvent. The implications of these interactions on dissolution efficiency, radiolytic stability, and overall process performance will be examined. These studies aim to underscore the importance of understanding radiation effects in the development of next-generation UNF reprocessing technologies and the global transition towards more sustainable and efficient nuclear energy systems.

38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL↗
DOE OSTI2022

Radiolytic evaluation of select sulfur chlorides (S 2 Cl 2 and SOCl 2 ) for advanced low temperature chlorination of zirconium-based used nuclear fuel cladding

New sulfur chloride compounds—sulfur monochloride (S 2 Cl 2 ) and thionyl chloride (SOCl 2 )—have been proposed as alternative chlorinating agents for the chemical decladding of zirconium-based used nuclear fuel cladding materials. However, the radiation stability of these compounds has not been thoroughly evaluated, despite envisioned process conditions involving intense, multi-component radiation fields. Knowledge of the radiation chemistry of these sulfur chlorides is essential for the development and optimization of alternative chlorination technologies. To this end, we present preliminary findings on the gamma radiolysis of neat S 2 Cl 2 and SOCl 2 at ambient temperature up to ~ 34 MGy. In this study, Raman spectroscopy and density functional theory calculations were used to identify the Raman-active degradation products from S 2 Cl 2 and SOCl 2 radiolysis. Both sulfur chloride compounds exhibited significant radiation resistance, with respect to changes in the Raman signatures of the parent compounds and the ingrowth of Raman-active degradation products. For S 2 Cl 2 , molecular chlorine (Cl 2 ) was directly identified as the predominant degradation product, which was completely consumed at higher absorbed doses (> 9 MGy). Similarly, the main degradation product from SOCl 2 radiolysis was also Cl 2 , although in this system it continued to grow in with dose over the entire dose range. Further, an “S=O” containing degradation product(s) was also identified as a compliment to Cl 2 . Overall, the perceived radiation resistance of these sulfur chloride compounds makes them suitable for inclusion in a used nuclear fuel chemical decladding process, especially as radiolytically formed Cl 2 can be used to reform the parent compounds, thereby increasing the longevity of the solvents used.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Gas-solid reaction pathway for chlorination of rare earth and actinide metals using hydrogen and chlorine gas

Hydriding and chlorination of buttons of metallic cerium have been tested as a head-end step to separating metal impurities from actinides. The objective here was to achieve complete conversion to chlorides while maintaining high surface area via small particles and open porosity. Hydriding by reaction with 100% H 2 gas at 573 K was successful at reducing cm-scale metal buttons into small particles/fragments. This step was followed by reaction with flowing 99.5% anhydrous Cl 2 gas at temperatures ranging from 423 to 573 K for 60 min. In experiments reported here, up to 92% conversion to cerium chloride was achieved from reacting with the anhydrous chlorine gas. The final chloride product has high porosity coupled with small particle sizes (microns to 1600 μm), which makes it suitable for subsequent purification processes. Higher chlorine concentrations in the gas favor higher conversion to chloride. The optimal temperature to achieve high chlorination is 523 K. Oxygen is a minor impurity in the chlorine gas which appears to prevent complete chlorination from being achieved.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Chlorination of Hydrogenated Silicon Nanosheets Revealed by Solid-State Nuclear Magnetic Resonance Spectroscopy

We report two-dimensional silicon nanosheets (Si-NS) synthesized by topotactic deintercalation of CaSi 2 are hypothesized to consist of buckled layers of sp 3 -hybridized silicon atoms that are bonded to three other framework Si atoms and a terminal atom or functional group such as H, Cl, or OH. Here, we apply 1 H{ 35 Cl} and 29 Si{ 35 Cl} Resonance-Echo Saturation-Pulse DOuble-Resonance (RESPDOR) solid-state NMR experiments to directly confirm the presence of chlorinated Si atoms within Si-NS. Plotting the 1 H{ 35 Cl} RESPDOR dephasing as a function of the 35 Cl saturation pulse offset reveals that the 35 Cl quadrupolar coupling constant (C Q ) is 38 MHz, consistent with Cl atoms that are covalently bonded to silicon. Modeling the 1 H{ 35 Cl} RESPDOR dephasing curve shows that the Si–Si interlayer spacing is approximately 6 Å. Plane-wave density functional theory (DFT) calculations show that the direct band gap transition of the Si-NS decreases with increasing chlorination and hydroxylation, suggesting that the band gap of Si-NS can be tuned by modifying the terminal atoms or functional groups.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Sorption Behavior of Iodate Ions on Calcium Silicate Hydrate under a High Saline Condition - 18176

The sorption behavior of iodate ions on calcium-silicate hydrate (CSH) gel under high saline condition was examined by monitoring the concentrations of iodate ions and chloride ions using ion chromatography and Raman spectroscopy, without drying process. In the sorption experiments, a stable isotope I-127 was used as an alternative of I-129 which is radioactive one. Each sample was synthesized with mixing CaO powder, SiO{sub 2} as fumed silica and NaCl solution. Ca/Si molar ratios of CSH gel were set to 0.4, 0.8, 1.2 and 1.6 (add 0.2, 0.6, 1.0 and 1.4 only L/S = 20), and the concentration of NaCl solution was set to 0 M or 0.6 M for simulating the condition of fresh or saline groundwater. The liquid/solid (L/S) ratios of CSH gel were set to 10, 15 and 20, and the total weight of solid phase was 1.5 g. At the same time, NaIO{sub 3} solution was added to the sample in order to adjust its concentration to 1.0 mM, 0.67 mM and 0.5 mM for each L/S ratios. The synthesis procedure for all samples was conducted in a glove bag filled with nitrogen gas. The curing period was 7, 14, 30, and 60 days at a room temperature (298 K) with shaking at 120 strokes/min. As a results, the concentration of iodate ions in the liquid phase decreased for all samples under experimental conditions. Besides, the sorption behavior of iodate ions were hardly changed by the concentration of NaCl. That is, iodate ions migrated to solid phase in spite of the high concentration of NaCl. The distribution coefficients, Kd, increased as Ca/Si ratio increased, and hardly depended on NaCl concentration. The results of Raman analysis shows that the structure of CSH gel was almost not changed with or without NaCl from the viewpoint of the silicate chain under this condition. These results suggest that a sorption process except for the electrostatic process such as an ion exchange and a complexation exists between CSH gel and iodate ions. Besides, CSH gel might be able to contribute the retardation for the migration of iodate ions without changing its structure, even if the disposal environment are saturated by a high saline groundwater. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS1991

In situ measurements of midlatitude ClO in winter

In situ measurements of ClO in the winter lower stratosphere are presented for six flights of the NASA ER-2 aircraft from 38 deg N to 61 deg N. Enhanced abundances, increasing in severity with date, were observed below 20 km, where HCl and ClONO2 dominate the inorganic chlorine budget. The greatest mixing ratios, over 150 pptv, were encountered on February 20 and 21, 1989, as the vortex experienced a major warming. Although the timing of these ClO enhancements and the evidence that vortex air can reach midlatitudes suggest that heterogeneous conversion of chlorine compounds within the vortex influences chemistry at midlatitudes, the enhacements observed early in the winter could have been caused by unknown chemistry occurring outside the vortex. In either case, photochemical loss of ozone due to catalytic reactions involving ClO at these mixing ratios may be responsible in part for the ozone decreases observed at high latitudes in the Northern Hemisphere.

Toohey, D. W.↗
DOE OSTI2025

Impacts of Ionizing Radiation on Sulfur Chloride Compounds for Advanced Fuel Cladding Decontamination Processes

Tripling the nation’s nuclear energy capacity is a critical component for significantly increasing energy production and reducing energy costs for American families and businesses. Achieving this vision requires fuel cycle technologies that maximize resource utilization while minimizing radioactive waste generation. Advanced sulfur chloride–based chlorination technologies are being developed to enable efficient recycling of fuel cladding materials, which account for a significant fraction of used nuclear fuel. However, the impacts of ionizing radiation on the longevity and performance of these sulfur chloride compounds are not well established. Here, we will explore the effects of gamma and electron-beam irradiation on the chemical composition of select sulfur chloride reagents, specifically sulfur monochloride (S2Cl2) and thionyl chloride (SOCl2), and the impacts of pre-irradiation on the chlorination yield/chemical dissolution of surrogate aluminum alloy 6061 (AA6061-T6) materials.

38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL↗
NASA NTRS1985

Stratospheric ClO - In-situ detection with a new approach

Stratospheric chlorine monoxide concentrations were measured in situ using a new and improved observational method in which the detection package is lowered on a tether from a balloon-borne platform floating near 40 km altitude and then reeled back up. Two reel down and reel up sequences covering 38 to 31 km produced (ClO) profiles which agree with each other to + or - 12 percent. The measured (ClO) profile falls within the envelope of nine previous fast parachute drop results, but exhibits a different shape, peaking near 32 km as opposed to approximately 39 km for the average of the previous profiles. These results are lower than but consistent with the profiles derived from remote sensing methods, and indicate the need for simultaneous measurements of relevant species.

Brune, Wm. H.↗