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At least 1,081 records · Page 60
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Equilibrium, Kinetic and Thermodynamic Studies on Methylene Blue Adsorption by Konjac Glucomannan/Activated Carbon Aerogel

Activated carbon (AC) is a common adsorbent used for the purification of aqueous solutions, yet its poor aqueous dispersion may negatively affects its practicability significantly. In the present study, the fabrication of an AC aerogel immobilized with konjac glucomannan (KGM/AC) for environmental protection was reported, and the parameters (e.g. AC content in aerogel, solution pH, adsorption duration, adsorption temperature and adsorbent dosage) were analyzed systematically using methylene blue (MB) as a model adsorbate. Further, to explore the adsorption equilibrium isotherm at equilibrium, the adsorption data were respectively fitted to Langmuir and Freundlich models, while kinetics study was conducted to explain the adsorption mechanism and predict the adsorption efficiency. Besides, the effect of temperature on the adsorption behavior was assessed using Van’t Hoff equation. According to the experimental and calculative results, the adsorption data at equilibrium could be well geared into the Langmuir model, and the adsorption kinetics behavior was better consistent with the pseudo-second-order expression as well as the intra-particle diffusion model. The Brunauer, Emmett and Teller surface area of KGM/AC aerogel was 352.44 m{sup 2}/g. KGM/AC aerogel exhibited the maximal capacity of adsorption of 416.67 mg/g at 323 K, and its adsorption behavior toward MB was endothermic and spontaneous in nature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

One-Pot Depolymerization and Polycondensation of PET Based Random Oligo- and Polyesters

The glycolysis of PET is a promising well-developed technique that could be utilized in a wide range of processes. Due to its equilibrial nature, the high ratio of reagents and the purification steps it is an expensive process. In this study our goal was to modify the standard glycolysis to an easily modulateable method (acido-alcoholysis) suited for one-pot oligoester, polyester synthesis. Adipic acid was added to the depolymerization reaction to connect low molecular weighed components into oligoesters. PET depolymerization reaction series were carried out with ethylene–glycol/adipic acid and butane-1,4-diol/adipic acid to demonstrate the tuneability of these systems. The reaction products were thoroughly characterized with NMR, FTIR, TGA, DSC and functional group analysis. One-pot depolymerization-polycondensation reactions were engineered to produce unsaturated and saturated polyesters. The unsaturated polyesters were dissolved in styrene, cross-linked and moulded to be characterized with DMA. A decreasing tendency of the glass transition temperature and cross-link density were found in the function of the ratio of adipic acid used during the depolymerization step. Acido-alcoholysis proved to be a versatile technique that could be used to engineer oligoesters and polyesters. The reagent use can be minimalized, and the raw reaction products can be directly applied as mid-products.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Californium Electrodepositions at Oak Ridge National Laboratory

Electrodepositions of californium isotopes were successfully performed at Oak Ridge National Laboratory (ORNL) during the past year involving two different types of deposition solutions, ammonium acetate (NH 4 C 2 H 3 O 2 ) and isobutanol ((CH 3 ) 2 CHCH 2 OH). A californium product that was decay enriched in 251 Cf was recovered for use in super-heavy element (SHE) research. This neutron-rich isotope, 251 Cf, provides target material for SHE research for the potential discovery of heavier isotopes of Z=118. The californium material was recovered from aged 252 Cf neutron sources in storage at ORNL. These sources have decayed for over 30 years, thus providing material with a very high 251 Cf-to- 252 Cf ratio. After the source capsules were opened, the californium was purified and then electrodeposited using the isobutanol method onto thin titanium foils for use in an accelerator at the Joint Institute for Nuclear Research in Dubna, Russia. Another deposition method, ammonium acetate, was used to produce a deposition containing 1.7 0.1 Ci of 252 Cf onto a stainless steel substrate. This was the largest single electrodeposition of 252 Cf ever prepared. The 252 Cf material was initially purified using traditional ion exchange media, such as AG50-AHIB and AG50-HCl, and further purified using a TEVA-NH 4 SCN system to remove any lanthanides, resulting in the recovery of 3.6 0.1 mg of purified 252 Cf. The ammonium acetate deposition was run with a current of 1.0 amp, resulting in a 91.5% deposition yield. Purification and handling of the highly radioactive californium material created additional challenges in the production of these sources.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2015

Production of ⁶¹Cu by the nat Zn(p,α) reaction: Improved separation and specific activity determination by titration with three chelators

In this study, the cyclotron-based production of position-emitting ⁶¹Cu using the (p,α) reaction at 11.7 MeV was investigated starting from natural-zinc ( nat Zn) and enriched ⁶⁴Zn-foil targets, as well as its subsequent purification. For nat Zn, a combination of three resins were assessed to separate ⁶¹Cu from contaminating 66,67,68 Ga and nat Zn. The specific activity of the purified ⁶¹Cu determined using ICP-MS analysis ranged from 143.3±14.3(SD) to 506.2±50.6 MBq/μg while the titration method using p-SCN-Bn-DOTA, p-SCN-Bn-NOTA and diamsar gave variable results (4.7±0.2 to 412.5±15.3 MBq/μg), with diamsar lying closest to the ICP-MS values. Results suggest that the p-SCN-Bn-DOTA and p-SCN-Bn-NOTA titration methods are significantly affected by the presence of trace-metal contaminants.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2015

Developing 226 Ra and 227 Ac age-dating techniques for nuclear forensics to gain insight from concordant and non-concordant radiochronometers

The model age or ‘date of purification’ of a nuclear material is an important nuclear forensic signature. In this study, chemical separation and MC-ICP-MS measurement techniques were developed for 226 Ra and 227 Ac: grand-daughter nuclides in the 238 U and 235 U decay chains respectively. The 230 Th- 234 U, 226 Ra- 238 U, 231 Pa- 235 U, and 227 Ac- 235 U radiochronometers were used to calculate model ages for CRM-U100 standard reference material and two highly-enriched pieces of uranium metal from the International Technical Working Group Round Robin 3 Exercise. In conclusion, the results demonstrate the accuracy of the 226 Ra- 238 U and 227 Ac- 235 U chronometers and provide information about nuclide migration during uranium processing.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2016

Measurement Background and the Sediment Age-Dating Reach of 32Si

Silicon-32 has been identified as an isotope that fills the sediment geochronology gap created between Pb-210 at <150 years and C-14 at >1000 years. However, detector sensitivity and chemical isolation challenges of radiometric Si-32 for age dating have resulted in a fairly limited number of applications of this technique to real-world sediment studies. The significance of targeting the intermediate age bracket is to provide accurate geochronological reconstructions of paleoindicators that identify human and large-scale, climate-induced shifts in coastal areas. Therefore, we targeted Puget Sound, Washington, United States, to demonstrate the application of Si-32 age dating to determine the relative importance of climate cycles versus human activities in an in-land sea. The enhanced reconstructions will be achieved through the design of new detectors, chemical separation of biogenic silica from kilogram-scale sediment samples, and demonstration of the viable age-dating reach of Si-32. Implications of detector background on the duration of required measurements and the age-dating reach are considered. The design of a low-background, gas-proportional beta counter for measurement of the daughter isotope P-32 is discussed; detector background goals for these new detectors are based on the sensitivity study.

Keillor, Martin E.↗
DOE OSTI2015

A performance comparison of commercially available strontium extraction chromatography columns

Extraction chromatographic separations following a nuclear event will require both speed and accuracy. Ideally these separations will be carried out using commercially available products. Because 90Sr is a likely material to be used in a radioactivity dispersal device, commercially available products for the separation of strontium were tested to evaluate differences in their elution profiles that may affect elution procedures. Gravity flow columns show better resolution, but vacuum flow columns allow rapid processing and are still adequate for purification if multiple aqueous conditions can be employed in the elution strategy.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2017

Application of the 226 Ra– 230 Th– 234 U and 227 Ac– 231 Pa– 235 U radiochronometers to uranium certified reference materials

Uranium certified reference materials (CRM) issued by New Brunswick Laboratory were subjected to dating using four independent uranium-series radiochronometers. In all cases, there was acceptable agreement between the model ages calculated using the 231 Pa– 235 U, 230 Th– 234 U, 227 Ac– 235 U or 226 Ra– 234 U radiochronometers and either the certified 230 Th– 234 U model date (CRM 125-A and CRM U630), or the known purification date (CRM U050 and CRM U100). Finally, the agreement between the four independent radiochronometers establishes these uranium certified reference materials as ideal informal standards for validating dating techniques utilized in nuclear forensic investigations in the absence of standards with certified model ages for multiple radiochronometers.

226Ra↗
DOE OSTI2018

Integration of a hyphenated HPIC-ICPMS protocol for the measurement of transplutonium isotopic mass distributions for 252Cf campaigns at Oak Ridge National Laboratory

Rapid measurement of transplutonium isotopic mass distributions during 252Cf production campaigns at Oak Ridge National Laboratory is a critical need. Mass measurements for the isotopes of plutonium, americium, curium, and californium are routinely requested to support the α-hydroxy-isobutyrate runs for the purification and recovery of the heavy curium target material and final 249Bk, 252Cf, and 254Es enriched isotope products. This paper presents the integration of an online high-pressure ion chromatography inductively coupled plasma mass spectrometry technique together with the protocol and chemistry that allows for rapid baseline separation and direct quantification of the transplutonium elemental concentrations and isotopic compositions.

Roach, Benjamin↗
DOE OSTI2020

International cooperation in age-dating uranium standards for nuclear forensics using the 231 Pa/ 235 U radiochronometer

During 2017–2018 Los Alamos National Laboratory, Lawrence Livermore National Laboratory and the China Institute of Atomic Energy collaborated in an interlaboratory 231 Pa/ 235 U radiochronometry exercise. The laboratories used different analytical methods to obtain a consensus model purification date for CRM U010 of December 28, 1958 ± 198 days and for CRM U850 of May 20, 1958 ± 363 days. These results agree with previously reported model dates using the 230 Th/ 234 U radiochronometer as well as the production histories of these materials. The concordance of interlaboratory data here confirms the ability of laboratories to make reproducible radiochronometry measurements using distinct analytical approaches.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Impact of lowering potassium contamination in liquid scintillation cocktails for ultra-sensitive radiation detection

Intrinsic 40 K radioactive backgrounds from impurities of natural K in liquid scintillation cocktails have previously been demonstrated to limit their use in ultra-sensitive applications. Here, this work explores two methodologies in parallel for the reduction of 40 K backgrounds in the cocktails, and lays the groundwork for use in ultra-sensitive applications. In one method, alternative low-K liquid scintillation matrix constituents were identified and in the other, a simple purification method for single components and finished cocktails was developed. Both methods were verified via ICP-MS analysis. Liquid scintillation counting of selected purified cocktails demonstrated background reduction, improved stability, and enhanced performance. The best performing purified cocktail was also counted on a custom-built ultra-low background liquid scintillation counter, with results below the detector background.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Cation exchange separation of radium and actinium using lactic acid DTPA buffer

The separation of actinium ( 228 Ac) from radium ( 223,228 Ra) on cation exchange resin with a diethylenetriaminpentaacetic acid-lactate buffer solution is demonstrated with series of columns. High yield, high radiopurity (~ 100%) separations of Ac from Ra are feasible with small columns in biologically compatible conditions and pHs. As Ac is eluted before Ra on these columns, further studies were performed to determine if this separation system could be applied to Ra/Ac isotope generators, but these were not successful. In conclusion, the separations presented in this work may be relevant for radiopharmaceutical purifications of 225 Ac which is typically obtained from its 225 Ra parent isotope.

and nuclear chemistry↗
DOE OSTI2026

Radioisotope dating of nuclear materials using cryogenic decay energy spectrometry

Cryogenic decay energy spectrometry provides high energy resolution and enables absolute decay counting, offering an alternative measurement technique for radiochronometry. A cryogenic decay energy spectrometry experiment was conducted using a magnetic microcalorimeter to determine the age of a plutonium sample. The energy resolution was measured at 0.05% from 5 to 6 MeV. The time since sample purification was determined using the measured concentration ratio of the 241 Am/ 241 Pu radiochronometer. Sample age estimates based on 241 Pu alpha-decay and beta-decay counts, along with 241 Am decay counts, align with the expected sample age within expanded uncertainty (k = 2), supporting the accuracy of cryogenic decay energy spectrometry as a radiochronometric method.

and nuclear chemistry↗
DOE OSTI2022

Biochemical and spectroscopic characterizations of the oligomeric antenna of the coral symbiotic Symbiodiniaceae Fugacium kawagutii

Light-harvesting antennas in photosynthesis capture light energy and transfer it to the reaction centers (RCs) where photochemistry takes place. The sustainable growth of the reef-building corals relies on a constant supply of the photosynthates produced by the endosymbiotic dinoflagellate, belonging to the family of Symbiodiniaceae. The antenna system in this group consists of the water-soluble peridinin-chlorophyll $\textit{a}$-protein (PCP) and the intrinsic membrane chlorophyll $\textit{a}$-chlorophyll $c_2$-peridinin protein complex (acpPC). In this report, a nonameric acpPC is reported in a dinoflagellate, Fugasium kawagutii (formerly Symbiodinium kawagutii sp. CS-156). We found that extensive biochemical purification altered the oligomerization states of the initially isolated nonameric acpPC. The excitation energy transfer pathways in the acpPC nonamer and its variants were studied using time-resolved fluorescence and time-resolved absorption spectroscopic techniques at 77 K. Compared to the well-characterized trimeric acpPC, the nonameric acpPC contains an 11 nm red-shifted terminal energy emitter and substantially altered excited state lifetimes of Chl $\textit{a}$. The observed energetic overlap of the fluorescence terminal energy emitters with the absorption of RCs is hypothesized to enable efficient downhill excitation energy transfer. Additionally, the shortened Chl $\textit{a}$ fluorescence decay lifetime in the oligomeric acpPC indicate a protective self-relaxation strategy. We propose that the highly-oligomerized acpPC nonamer represents an intact functional unit in the Symbiodiniaceae thylakoid membrane. They perform efficient excitation energy transfer (to RCs), and are under manageable regulations in favor of photoprotection.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2018

Alpha-Emitters and Targeted Alpha Therapy in Oncology: from Basic Science to Clinical Investigations

Alpha-emitters are radionuclides that decay through the emission of high linear energy transfer α-particles and possess favorable pharmacologic profiles for cancer treatment. When coupled with monoclonal antibodies, peptides, small molecules, or nanoparticles, the excellent cytotoxic capability of α-particle emissions has generated a strong interest in exploring targeted α-therapy in the pre-clinical setting and more recently in clinical trials in oncology. Multiple obstacles have been overcome by researchers and clinicians to accelerate the development of targeted α-therapies, especially with the recent improvement in isotope production and purification, but also with the development of innovative strategies for optimized targeting. Numerous studies have demonstrated the in vitro and in vivo efficacy of the targeted α-therapy. Radium-223 ( 223 Ra) dichloride (Xofigo®) is the first α-emitter to have received FDA approval for the treatment of prostate cancer with metastatic bone lesions. There is a significant increase in the number of clinical trials in oncology using several radionuclides such as Actinium-225 ( 225 Ac), Bismuth-213 ( 213 Bi), Lead-212 ( 212 Pb), Astatine ( 211 At) or Radium-223 ( 223 Ra) assessing their safety and preliminary activity. Finally, this review will cover their therapeutic application as well as summarize the investigations that provide the foundation for further clinical development.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2018

Interaction Between Liquid Silver and Graphene-Coated SiC Substrate

Wettability between liquid Ag and graphene-coated SiC single crystal has been investigated by dispensed drop method at T = 970 °C under vacuum accompanied with subsecond recording of the drop/substrate images (100 frames per second) by high-speed high-resolution CCD camera. Non-contact heating method coupled with capillary purification of the Ag drop procedure has been applied. Scanning electron microscopy combined with EDS analysis and scanning probe microscopy combined with Raman spectroscopy techniques has been utilized for microstructure and surface characterization of samples before and after high-temperature wetting tests. Immediately after its detachment from the capillary, the Ag drop showed non-wetting behavior (θ > 90°) forming a high contact angle of θ = 114°. Surface characterization of the drop surface after wettability tests evidenced the presence of graphene and Si transferred from the substrate to the top of Ag drop. These findings suggest chemical interaction phenomena occurring at the interface. Locally, an intimate contact between liquid Ag and SiC substrate was allowed by the appearance of discontinuities in the graphene layer basically produced by thermomechanical stress. Local dissolution of carbon into liquid Ag and its reorganization (by segregation, nucleation and growth) as secondary graphene layer at the Ag surface was also observed.

36 MATERIALS SCIENCE↗
DOE OSTI2019

A Study of the Activity of Recombinant Mn-Superoxide Dismutase in the Presence of Gold and Silver Nanoparticles

Superoxide dismutase (SOD) is one of the best characterized enzyme maintaining the redox state in the cell. A bacterial expression system was used to produce human recombinant manganese SOD with a His-tag on the C-end of the protein for better purification. In addition, gold and silver nanoparticles were chemically synthesized in a variety of sizes, and then mixed with the enzyme for immobilization. Analysis by dynamic light scattering and scanning transmission electron microscopy revealed no aggregates or agglomerates of the obtained colloids. After immobilization of the protein on AuNPs and AgNPs, the conjugates were analyzed by SDS-PAGE. It was determined that SOD was adsorbed only on the gold nanoparticles. Enzyme activity was analyzed in colloids of the gold and silver nanoparticles bearing SOD. The presence of a nanoparticle did not affect enzyme activity; however, the amount of protein and size of the gold nanoparticle did influence the enzymatic activity of the conjugate. Our findings confirm that active recombinant human superoxide dismutase can be produced using a bacterial expression system, and that the enzyme can be immobilized on metal nanoparticles. The interaction between enzymes and metal nanoparticles requires further investigation.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2023

Selective Pb 2+ removal and electrochemical regeneration of fresh and recycled FeOOH

Heavy metal pollution is a key environmental problem. Selectively extracting heavy metals could accomplish water purification and resource recycling simultaneously. Adsorption is a promising approach with a facile process, adaptability for the broad concentration of feed water, and high selectivity. However, the adsorption method faces challenges in synthesizing high-performance sorbents and regenerating adsorbents effectively. FeOOH is an environmentally friendly sorbent with low-cost production on a large scale. Nevertheless, the selectivity behavior and regeneration of FeOOH are seldom studied. Therefore, we investigated the selectivity of FeOOH in a mixed solution of Co 2+ , Ni 2+ , and Pb 2+ and proposed to enhance the capacity of FeOOH and regenerate it by using external charges. Without charge, the FeOOH electrode shows a Pb 2+ uptake capacity of 20 mg/g. After applying a voltage of –0.2/+0.8 V, the uptake capacity increases to a maximum of 42 mg/g and the desorption ratio is 70%–80%. In 35 cycles, FeOOH shows a superior selectivity towards Pb 2+ compared with Co 2+ and Ni 2+ , with a purity of 97% ± 3% in the extracts. The high selectivity is attributed to the lower activation energy for Pb 2+ sorption. The capacity retentions at the 5 th and the 35 th cycles are ca. 80% and ca. 50%, respectively, comparable to the chemical regeneration method. With industrially exhausted granular ferric hydroxide as the electrode material, the system exhibits a Pb 2+ uptake capacity of 37.4 mg/g with high selectivity. Our work demonstrates the feasibility of regenerating FeOOH by charge and provides a new approach for recycling and upcycling FeOOH sorbent.

36 MATERIALS SCIENCE↗