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At least 1,117 records · Page 62
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Assessment the leaching characteristics and long-term leaching behavior of some radionuclides from synthesized zeolite cement matrix

Highlights: • Synthesis and characterization of zeolite cement synthesized from fly ash • Leaching tests were used to assess the release rate of {sup 85}Sr and {sup 60}Co radionuclides. • Simple mathematical models were used to detect leaching mechanisms. • Long-term leaching behavior of {sup 85}Sr and {sup 60}Co from cementitious matrix was assessed. The development of cementitious materials remains a vital goal to produce valuable products with good mechanical, physical and chemical properties suitable for the safe disposal of concentrated radionuclides resulted from the treatment of contaminated solutions. In this paper, zeolite cement with good properties was laboratory synthesized from industrial by-products fly ash and characterized using various characterization techniques. The leaching characteristics of strontium and cobalt radionuclides from the synthesized zeolite cement were scrutinized conforming with the standard leaching methodology of International Atomic Energy Authority (IAEA). A mechanical strength assessment was executed to characterize the extent of immobilization process of the solidified matrices. The cumulative leaching fraction (φ) of the two studied radionuclides was found to be less than 5% in all examined conditions, which implies the applicability of the IAEA-recommended methodology for estimating the diffusion coefficient. The experimental leaching data were regressed nonlinearly to various mathematical kinetic models to assess the controlling leaching mechanism and to determine the leaching parameters. The regression results indicated that strontium ({sup 85}Sr) and cobalt ({sup 60}Co) leaching resulted from two succeeding mechanisms: as first order kinetic reaction, and then diffusion. The calculated values of leachability indices signify that the performance of each of the studied matrices is within an acceptable range. A simplified mathematical model, rooted in the first order reaction and diffusion mechanisms, was simulated to predict the radionuclides leaching rates from zeolite cement matrices. By comparing the synthesized zeolite cement with other cementitious materials, it can be concluded that the synthesized material can be classified as an efficient material suitable to immobilize {sup 85}Sr and {sup 60}Co from radioactive wastes. The acquired findings demonstrated that the studied immobilized waste matrices have acceptable mechanical effectiveness.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Understanding of the factors slowing down metakaolin reaction in limestone calcined clay cement (LC3) at late ages

Factors which could explain the slowing down of the metakaolin reaction in LC{sup 3} blends are investigated. Portlandite availability and the presence of aluminium ions in the pore solution are shown not to be limiting factors. Hydrates can only precipitate in solution filled pores. Internal relative humidity measurements indicate that at 28 days solution is present only in pores with radii below 13 nm. An enhancement of metakaolin reaction was obtained at late ages when the larger capillaries are filled with solution. The lower limit of the water filled pores was more difficult to analyse since there is a lack of precision in determining interfacial energies of hydrates and pore solution of the system. However, this study gives an indication of order of magnitude where the growth of hydrates could be slowed down.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Screening candidate supplementary cementitious materials under standard and accelerated curing through time-series surface resistivity measurements and change-point detection

Time-series surface resistivity (SR) measurements are evaluated as an indicator of pozzolanicity in concretes containing 13 materials of both known and unknown pozzolanicity, under standard and accelerated curing conditions, and the results were validated against portlandite consumption obtained through thermogravimetric analysis. Change-point detection (CPD) analysis is applied to the data to provide a rigorous indicator of hydration age of the onset and rate of the pozzolanic reaction, if occurring. The SR measurements were able to capture the onset of the pozzolanic reactions in concretes curing at elevated temperature regimes, which allows determination of pozzolanicity weeks earlier than at standard curing temperatures. Using CPD along with slope analysis allows a comprehensive analysis of a material's reactivity and determination of pozzolanicity in as quickly as two days. Time-series SR measurements at elevated curing conditions, along with limits on material composition, are recommended for determination of pozzolanic reactivity in novel or variable materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Ultra-high gamma irradiation of calcium silicate hydrates: Impact on mechanical properties, nanostructure, and atomic environments

The concrete biological shield in a nuclear power plant receives ~100–200 MGy gamma dosage during an 80-year design life. However, precise changes in the mechanical properties and atomic environments of C-S-H at ultrahigh irradiation dosages have not been systematically documented. Here, we report that irradiation decreases C-S-H basal spacing (~ 0.6 ± 0.1 Å for 189 MGy) and increases its Young's modulus, which is attributed to the lower basal spacing as the nano porosity potentially increased and microporosity remained unchanged. Irradiation also decreased the molecular water content and increased hydroxyl groups in C-S-H, showing that interlayer water removal reduces the basal spacing. Finally, 1 H and 29 Si NMR results indicate some disorder in the local proton CaO-H species and slight depolymerization of the silicate structure. Together, these results indicate that the C-S-H gel stiffens upon ultrahigh gamma irradiation dosage, a finding which concerns long-term nuclear power plants operations worldwide.

1H NMR↗
DOE OSTI2024

Microstructural characterization and equibiaxial flexural strength of CeO 2 and Ti-doped CeO 2

In this study, the synthesis of CeO 2 and titanium dioxide (TiO 2 ) doped CeO 2 (TDC) monoliths are investigated, and their fracture strength is assessed using an equibiaxial flexure testing technique at room temperature. Pellets were synthesized using conventional powder processing and sintering methods to produce the desired characteristics. The TiO 2 dopant concentration was optimized at 0.1 wt % TiO 2 to obtain dense, solid-solution pellets with an enhanced grain microstructure. A ball-on-ring fixture was used to obtain the TRS and Weibull parameters of over 30 pellets for CeO 2 and 0.1 wt % TDC to compare fracture behavior. The TRS of CeO 2 pellets ranged from 88 to 160 MPa and the TRS of 0.1 wt % TDC pellets ranged from 102 to 171 MPa, both being consistent with published values. Weibull parameters, such as characteristic strength and Weibull modulus, were extracted as 129 MPa and 8.5 for CeO 2 and 150 MPa and 9.3 for 0.1 wt % TDC, respectively. Although Hertzian contact damage was observed on compressive surfaces, failure initiation occurred on the tensile surfaces of both types of samples. Fracture surface analysis for CeO 2 indicated a predominantly intergranular fracture while 0.1 wt % TDC had a predominantly transgranular fracture mode. Finally, the TRS of 0.1 wt % TDC resulted in increased Weibull parameters when compared to CeO 2 , indicating sample chemistry and microstructure impact mechanical behavior for these samples.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Upcycling mixed cathode materials to high-energy-density LiFe 0.75 Mn 0.25 PO 4

To address the demand for next-generation cathode materials with high energy density, upcycling LiFePO 4 into LiFe 0.75 Mn 0.25 PO 4 has attracted considerable attention. Nevertheless, existing strategies have yet to achieve both morphology and full elemental recovery under mild ambient conditions. Here, we report an upcycling route that can address this issue by combining leaching and a high-temperature treatment process. The upcycled LiFe 0.75 Mn 0.25 PO 4 exhibits enlarged lattice spacing and a high discharge plateau, and it delivers an energy density of 563.7 Wh/kg, 40.3 Wh/kg higher than recycled LiFePO 4 , which indicates the high value of the proposed upcycling strategy. At 1 C, LiFe 0.75 Mn 0.25 PO 4 also exhibits excellent cycling stability of 91% over 700 cycles. Techno-economic analysis also indicates impressive economic and environmental benefits, including 10.4% less raw materials usage and 12.2% less energy consumption and wastewater generation. This work demonstrates a scalable and economic upcycling strategy and provides a promising pathway for sustainable battery upcycling compatible with industrial conditions.

LMFP↗
DOE OSTI2020

Mineral-specific heterogeneous neptunium sorption onto geological repository rocks in oxic and anoxic conditions and various temperatures

Neptunium poses challenges for radioactive wastes management due to its long half-life and ingrowth from americium decay, as well as its high mobility in water in its oxidized forms. Np(V)-bearing aqueous solutions were contacted with polished and crushed gneiss and dolerite from the Yeniseisky site, Russia, which is under consideration as a location for an underground repository, both in oxic and anoxic conditions at 20 and 90 °C. Neptunium sorption on crushed gneiss and dolerite in oxic conditions at 20 °C was quite low, but increased substantially in anoxic conditions. Autoradiography on samples treated at 20 °C revealed that sorbed Np was associated mostly with dark colored iron-bearing minerals, and solvent extraction indicated partial reduction of Np(V) to Np(IV). Sorption of Np from aqueous solutions contacted with dolerite and gneiss at 90 °C was in all cases higher than at the lower temperature. Autoradiography of polished rock samples treated in anoxic conditions at 90 °C revealed that Fe-bearing minerals had 3–4 orders of magnitude more Np sorbed on them than the quartz and feldspar grains. X-ray photoelectron spectroscopy indicated this sorbed Np was present as NpO 2 . This study supports the concept that the geologic conditions present at the planned repository site will retard Np migration.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Mobilization of trace metals from caprock and formation rocks at the Illinois Basin – Decatur Project demonstration site under geological carbon dioxide sequestration conditions

One concern for geologic CO 2 sequestration is the potential leakage of CO 2 or CO 2 -saturated brine containing trace metals into overlying aquifers, which poses the risk of adversely affecting underground sources of drinking water. In this work, rock and brine samples collected in the Illinois Basin – Decatur Project (IBDP), a large-scale geological CO 2 sequestration demonstration project in Decatur, Illinois, USA, as well as synthetic brine samples were used to understand the mobilization of trace metals as a result of CO 2 –rock–brine interactions under IBDP-specific conditions (50 °C and 20.6 MPa). Rock sample characterization indicated that, at the IBDP site, trace metal concentrations were greatest in cap rock samples from the Eau Claire Formation, compared with those from formations above and below this Formation. The natural brine samples collected from the Mt. Simon Sandstone reservoir were highly reducing and saline, with trace metal concentrations up to 680 times greater than the U.S. Environmental Protection Agency-prescribed drinking water standards. Batch leaching experiments indicated that both trace metal mobilization from rock and immobilization from the brine occurred when high-pressure CO 2 was introduced into the rock-brine system. The amounts of metals mobilized from the rock generally accounted for <5% of the total metals in the rock, but for some metals, including Ni, Pb, and Tl, up to 63% of the metals in the rock were mobilized to the brine. Leaching of trace metals into synthetic brines was different from that into the natural brine. The results of this study provided current information on the trace element sources and will help in risk simulations and experimental design to further evaluate potential impact of leakage on groundwater quality, which is important for future GCS projects to consider for monitoring and containment assurance purposes.

58 GEOSCIENCES↗
DOE OSTI2023

Can Zn isotopes in sediments record past eutrophication of freshwater lakes? A pilot study at Lake Baldegg (Switzerland)

In this study, the speciation and isotopic composition of Zn were traced across the sediments of a freshwater lake that experienced one hundred years of strong eutrophication, in order to assess the potential of sedimentary Zn isotopes to record such an environmental disturbance. Here, the results indicate that the sedimentary Zn isotope signal varied with the change from pre-eutrophic to eutrophic conditions in the investigated lake. The average δ 66 Zn JMC value of the dominantly allochthonous lithogenic sediments deposited during the pre-eutrophic period was +0.27‰ ±0.05‰ (i.e. similar to the δ 66 Zn JMC value of +0.28‰ ±0.05‰ proposed for Bulk Silicate Earth), while enhanced autochthonous biochemical sedimentation during the eutrophic period resulted in significantly lower δ 66 Zn JMC values down to +0.04‰ ±0.06‰. Synchrotron-based X-ray absorption spectroscopy data revealed a concomitant change in Zn speciation from a dominant fraction of Zn in clay minerals during the pre-eutrophic period to a major fraction of Zn in ZnS during the eutrophic period. A linear regression relating the sedimentary Zn isotope signal to the fraction of Zn in ZnS indicated δ 66 Zn JMC values of +0.27‰ ±0.06‰ and 0.00‰ ±0.08‰ for Zn in clay minerals and in ZnS, respectively. The enrichment of light Zn in ZnS in the eutrophic sediments is tentatively attributed to enhanced biological uptake of light Zn in the water column, which resulted in an enhanced flux of organic-bound Zn towards the sediments and further transformation of organic Zn into ZnS upon biomass mineralization during early diagenesis. This hypothesis is in agreement with the fractionation towards lighter Zn reported for both biological uptake of Zn and ZnS precipitation. The results of this study emphasize the potential of sedimentary Zn isotopes to register past eutrophic periods in freshwater lakes, and thus to serve as a probe of paleo-environmental conditions and/or past land use at the catchment scale.

58 GEOSCIENCES↗
DOE OSTI2023

Optimized thermodynamic properties of REE aqueous species (REE 3+ and REEOH 2+ ) and experimental database for modeling the solubility of REE phosphate minerals (monazite, xenotime, and rhabdophane) from 25 to 300 °C

Rare earth elements (REE) are critical elements found in monazite, xenotime, and hydrated REE phosphates which typically form in hydrothermal mineral deposits. Accurate predictions of the solubility of these REE phosphates and the speciation of REE in aqueous fluids are both key to understanding the controls on the transport, fractionation, and deposition of REE in natural systems. Previous monazite and xenotime solubility experiments indicate the presence of large discrepancies between experimentally derived solubility constants versus calculated solubilities by combining different data sources for the thermodynamic properties of minerals and aqueous species at hydrothermal conditions. In this study, these discrepancies were resolved by using the program GEMSFITS to optimize the standard partial molal Gibbs energy of formation (Δ f G° 298 ) of REE aqueous species (REE 3+ and REE hydroxyl complexes) at 298.15 K and 1 bar while keeping the thermodynamic properties fixed for the REE phosphates. A comprehensive experimental database was compiled using solubility data available between 25 and 300 °C. The latter permits conducting thermodynamic parameter optimization of Δ f G° 298 for REE aqueous species. Optimal matching of the rhabdophane solubility data between 25 and 100 °C requires modifying the Δ f G° 298 values of REE 3+ by 1–6 kJ/mol, whereas matching of the monazite solubility data between 100 and 300 °C requires modifying the Δ f G° 298 values of both REE 3+ and REEOH 2+ by ~15–31 kJ/mol and ~2–10 kJ/mol, respectively. For xenotime, adjustments of Δ f G° 298 values by 1–26 kJ/mol are only necessary for the REE 3+ species. The optimizations indicate that the solubility of monazite in acidic solutions is controlled by the light (L)REE 3+ species at <150 °C and the LREEOH 2+ species at >150 °C, whereas the solubility of xenotime is controlled by the heavy (H)REE 3+ species between 25 and 300 °C. Based on the optimization results, we conclude that the revised Helgeson-Kirkham-Flowers equation of state does not reliably predict the thermodynamic properties of REE 3+ , REEOH 2+ , and likely other REE hydroxyl species at hydrothermal conditions. We therefore provide an experimental database (ThermoExp_REE) as a basic framework for future updates, extensions with other ligands, and optimizations as new experimental REE data become available. As a result, the optimized thermodynamic properties of aqueous species and minerals are available open access to accurately predict the solubility of REE phosphates in fluid-rock systems.

58 GEOSCIENCES↗
DOE OSTI2025

Spectrophotometric determination of the stability of La hydroxyl complexes at near neutral to alkaline pH from 25 to 75 °C

The hydrolysis of rare earth elements (REE) potentially controls their mobility during fluid-rock interaction in a broad range of pH and temperature conditions. However, there is still a lack of thermodynamic data for modeling accurately the stability of REE hydroxyl complexes in hydrothermal aqueous fluids. Here, in this study, UV–Vis spectrophotometric experiments were conducted from 25 to 75 °C in near-neutral to alkaline NaOH-bearing aqueous solutions with varying lanthanum (La) concentrations (0 to ∼0.23 mmol/kg). The color indicator m-cresol purple was used to determine in situ pH and derive the average OH− ligand number ($\overrightarrow{n}$) and formation constants for the La hydroxyl complexes (LaOH 2+ , La(OH) 2 + , and La(OH) 3 0 ). From 25 to 50 °C, $\overrightarrow{n}$ ranges between ∼1 and 2 at pH from 7.0 to 9.3. At 75 °C, $\overrightarrow{n}$ ranges between ∼1.5 and 3 at pH from 6.3 to 8.8. These results suggest the predominance of LaOH 2+ and La(OH) 2 + complexes from 25 to 50 °C, and an increased predominance of La(OH) 3 0 at 75 °C. The cumulative formation constants (β n °, n = 1 to 3) are derived for the reaction La 3+ + nOH − = La(OH) n 3-n , and fitted between 25 and 250 °C by combining the UV–Vis and literature solubility data. The resulting logβ n ° are expressed as function of temperature (T in Kelvin): logβ 1 ° = −1.786 + 0.0133 T + 1.049·10 3 /T; logβ 2 ° = −5.797 + 0.0267 T + 2.713·10 3 /T; logβ 3 ° = 6.435 + 0.0223 T + 512.7/T. A comparison between these new fits and existing extrapolations using the Helgeson-Kirkham-Flowers equation of state indicates significant differences in the predicted hydrolysis of La. The latter extrapolations should therefore be updated for the hydrolysis of REE.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Impacts of anthropogenic gadolinium on the activity of the ammonia oxidizing bacterium Nitrosomonas europaea

Widespread use of gadolinium-based contrast agents in medical imaging has resulted in increased Gd inputs to municipal wastewater treatment plants. Others have reported that typical wastewater treatment does not attenuate Gd, resulting in discharges to natural waters. However, whether elevated Gd impacts the performance of biological treatment has not been investigated. We examined whether gadolinium chloride or Gd chelated with diethylenetriaminepentaacetic acid (DTPA) affected the activity of the model nitrifying bacterium Nitrosomonas europaea. At nominal GdCl 3 additions ranging from 1 to 500 µM, no impact was observed compared to the control. Most (>98%) of the added Gd precipitated, and extracellular GdPO 4 nanoparticles were observed. When chelated with DTPA, Gd remained soluble, but no statistically significant impact on ammonia oxidation was observed until the highest concentrations tested. At 300 and 500 µM Gd-DTPA, a temporary reduction of nitrite production relative to the control (effect size 1.3 mg l -1 and 1.5 mg l -1 , respectively, at 24 h) was seen. By itself, DTPA was highly inhibitory. Modeling suggested that DTPA likely chelated other metals, but adjusting the concentrations of the most abundant metals in the medium, calcium and magnesium, indicated that lowering their free ion activities was probably not the cause of inhibition. Complexation of other essential metals was more likely. Furthermore, our studies indicate that while the low bioavailability of Gd may limit its ecosystem impacts, the role of synthetic ligands used with Gd and other rare earth elements should e considered as the production, use and disposal of these elements increases.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Influence of ethylenediaminetetraacetic acid on the long-term oxidation state distribution of plutonium

Here, spectrophotometry was used to study the effect of EDTA on plutonium oxidation state distribution as a function of time, pH, and ligand-to-metal ratio (L/M) under anoxic conditions. Novel Pu(V)-EDTA absorption bands were identified at 571, 993, 1105, and 1150 nm with molar absorption coefficients of 15 ± 1, 6 ± 1, 10 ± 1, and 10 ± 1 cm –1 M –1 , respectively. Pu(V)-EDTA spectral changes occurred at L/M < 1, indicating only Pu V O 2 (EDTA) 3- formed with logK = 3.6 ± 0.3. Time-resolved experiments showed EDTA drastically increased the Pu(V/VI) reduction rate, which we propose is driven by amine lone-pair electron donation and the oxidative decarboxylation of EDTA. Oxidation of Pu(III)-EDTA to Pu(IV)-EDTA occurred on a slower time scale (110–237 days) than previously reported (<15 min) and is hypothesized to be radiolysis driven. Pu(V/VI)-EDTA and Pu(III)-EDTA both approached Pu(IV)-EDTA stabilization over time, yet Pu(V/VI)-EDTA solubility data was ≥ 1.0 log 10 units higher than predicted by Pu(IV)-EDTA solubility models, indicating that current thermodynamic models are incomplete. Ultimately, the data show EDTA preferentially stabilizes Pu(IV) over time regardless of initial oxidation state, but Pu(V)-EDTA can persist under environmentally-relevant conditions, emphasizing the need to continue investigating redox reactions, speciation, and behavior of these complexes to support the transuranic waste disposal and surface remediation/containment efforts.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Plutonium mobilization from contaminated estuarine sediments, Esk Estuary (UK)

Since 1952, liquid radioactive effluent containing 238-242 Pu, 241 Am, 237 Np, 137 Cs, and 99 Tc has been released with authorization from the Sellafield nuclear complex (UK) into the Irish Sea. This represents the largest source of plutonium (Pu) discharged in all western Europe, with 276 kg having been released. In the Eastern Irish Sea, the majority of the transuranic activity has settled into an area of sediments (Mudpatch) located off the Cumbrian coast. Radionuclides from the Mudpatch have been re-dispersed via particulate transport in fine-grained estuarine and intertidal sediments to the North-East Irish Sea, including the intertidal saltmarsh located at the mouth of the Esk Estuary. Saltmarshes are highly dynamic systems which are vulnerable to external agents (sea level change, erosion, sediment supply, and freshwater inputs), and their stability remains uncertain under current sea level rise projections and possible increases in storm activity. In this work, we examined factors affecting Pu mobility in contaminated sediments collected from the Esk Estuary by conducting leaching experiments under both anoxic and oxic conditions. Here, leaching experiments were conducted over a 9-month period and were periodically sampled to determine solution phase Pu via multicollector-inductively coupled plasma-mass spectrometry (MC-ICP-MS), and to measure redox indicators (Eh, pH and extractable Fe(II)). Microbial community composition was also characterized in the sediments, and at the beginning and end of the anoxic/oxic experiments. Results show that: 1) Pu leaching is about three times greater in solutions leached under anoxic conditions compared to oxic conditions, 2) the sediment slurry microbial communities shift as conditions change from anoxic to oxic, 3) Pu leaching is enhanced in the shallow sediments (0–10 cm depth), and 4) the magnitude of Pu leached from sediments is not correlated with total Pu, indicating that the biogeochemistry of sediment-associated Pu is spatially heterogeneous. These findings provide constraints on the stability of redox sensitive Pu in biogeochemically dynamic/transient environments on a timescale of months and suggests that anoxic conditions can enhance Pu mobility in estuarine systems.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

A comparative TEA of a two-step process using chemical solvents for producing an ultra-sweet natural gas

Here, a comprehensive Techno-Economic Analysis (TEA) was performed to evaluate the economic feasibility of a novel two-step process (TSP) developed in Aspen Plus V12.1 to desulfurize and decarbonize a raw natural gas containing (2 mol% H 2 S and 5 mol% CO 2 ) into an ultra-sweet natural gas containing (1.72 ppmv H 2 S and 4.19 ppmv CO 2 ). The raw natural gas flow rate used in the TSP was 117.74 kg/s at 60 °C and 50 bar. The TSP combines an H 2 S desulfurization step using potassium carbonate (K 2 CO 3 ) and a CO 2 capture step using 3 different chemical solvents, monoethanolamine (MEA), sodium glycinate (SGS), and potassium glycinate (PGS). Both steps employ fixed-bed absorbers packed with Mellapak 250Y structured packing. The hydraulics and mass transfer characteristics for the TSP were calculated, indicating normal operation with higher gas-side (k G ) than liquid-side (k L ) mass transfer coefficients. The TEA of TSP indicated that PGS had the most promising economic feasibility among the 3 solvents as it exhibited the lowest Levelized Cost of CO 2 capture (LCOC) of $\$$47.54/ton.CO 2 at a Capital Expenditure (CAPEX) of $\$$24.98 million, and an Operating Expenditure (OPEX) of $\$$12.20 million/year. Also, the TSP could produce one MMSCF of ultra-sweet natural gas at a total cost of $\$$339.55.

03 NATURAL GAS↗
DOE OSTI2021

Pre-existing humoral immunity to human common cold coronaviruses negatively impacts the protective SARS-CoV-2 antibody response

SARS-CoV-2 infection causes diverse outcomes ranging from asymptomatic infection to respiratory distress and death. A major unresolved question is whether prior immunity to endemic, human common cold coronaviruses (hCCCoVs) impacts susceptibility to SARS-CoV-2 infection or immunity following infection and vaccination. Therefore, we analyzed samples from the same individuals before and after SARS-CoV-2 infection or vaccination. We found hCCCoV antibody levels increase after SARS-CoV-2 exposure, demonstrating cross-reactivity. However, a case-control study indicates that baseline hCCCoV antibody levels are not associated with protection against SARS-CoV-2 infection. Rather, higher magnitudes of pre-existing betacoronavirus antibodies correlate with more SARS-CoV-2 antibodies following infection, an indicator of greater disease severity. Additionally, immunization with hCCCoV spike proteins before SARS-CoV-2 immunization impedes the generation of SARS-CoV-2-neutralizing antibodies in mice. Together, these data suggest that pre-existing hCCCoV antibodies hinder SARS-CoV-2 antibody-based immunity following infection and provide insight on how pre-existing coronavirus immunity impacts SARS-CoV-2 infection, which is critical considering emerging variants.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2023

Separation of rare earth element radioisotopes by reverse-phase high-speed counter-current chromatography

Analytical scale purification of rare earth element (REE) radioisotopes is typically accomplished using cation-exchange resins (e.g. AG 50W-X8) and high-performance liquid chromatography (HPLC). Despite the variety of improvements made since the development of this separation process in the 1950s, nearest neighbor separations remain a challenge, as does the issue of irreversible sample adsorption. Herein, we report a study that evaluates the potential of high-speed counter-current chromatography (HSCCC) as an alternative method for purifying REE elements, with specific reference to separations of fission product REE of interest to nuclear forensics. Complementary HSCCC REE separation experiments, one spiked with radiotracer and REE fission product activity, allowed for in depth analysis of resulting fractions from both an elemental (inductively coupled plasma atomic emission spectroscopy, ICP-AES) and radiological (gamma-ray spectrometry, beta counting) purity perspective. The highly reproducible nature of separation profiles generated from HSCCC instruments was leveraged to simplify work-up of samples containing radioisotopes. Subsequent radioanalytical evaluation revealed minimal carryover of Eu into neighboring Sm and Tb fractions (as indicated by presence of 150Eu), and trace contamination of the Tb fraction with Y (as indicated by presence of 91Y). Subtle differences in stationary phase retention across the two columns were reflected in significant variations in decontamination factors of duplicate parallel separations. Furthermore, these differences paired with obtained distribution of radioisotopes provided valuable insights into future improvements. Collectively, this study represents a significant step forward in development of HSCCC technology for task specific REE radioisotope purification.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2026

Evaluation of chromatographic resins for high efficacy separation of radium from chemical analogues

The separation of Radium (Ra) from interfering chemical analogues is of major importance for both the accurate measurement of Ra-226 in environmental samples and the preparation of radium targets destined for medical isotope production. The adsorption behavior of Ra, Barium (Ba), and Strontium (Sr) was investigated on multiple crown-ether-based proprietary extraction chromatographic resins developed by TrisKem Int. Among these, the TK101 resin, characterized by a novel room-temperature ionic liquid (RTIL) dual extractant–solvent system, demonstrated enhanced affinity and selectivity, particularly at low acid concentrations, achieving a D w of 3477 ± 73 for Ra in 0.04 M HNO₃, whereas the maximum Ra D w obtained with the traditional Sr resin in 8 M HNO 3 was only 12.33 ± 0.4. In 0.04 M HNO 3 , a Ra distribution ratio (D w ) of 776 was achieved within 1 min, indicating rapid uptake kinetics. The adsorption capacities were estimated at 19.6 ± 0.1 mg/g for Ba and 12.0 ± 0.2 mg/g for Sr. However, competing alkali metals significantly reduced alkaline earth metal uptake, indicating that the TK101 resin is best suited for radium purification following a preconcentration step to minimize matrix effects in high salinity samples. Dynamic column studies confirmed the strong chromatographic performance of the TK101 resin, with no significant Ba or Sr breakthrough in the Ra fraction and a Ra recovery of 87 ± 2.8%. These results demonstrate the potential of the TK101 resin for selective radium separation in analytical and radiochemical applications.

and nuclear chemistry↗