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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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12 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Evidence for Enhanced Tracer Diffusion in Densely Packed Interfacial Assemblies of Hairy Nanoparticles

Nearly monodisperse nanoparticle (NP) spheres attached to a nonvolatile ionic liquid surface were tracked by in situ scanning electron microscopy to obtain the tracer diffusion coefficient D tr as a function of the areal fraction Φ. The in situ technique resolved both tracer (gold) and background (silica) particles for ~1–2 min, highlighting their mechanisms of diffusion, which were strongly dependent on Φ. Structure and dynamics at low and moderate Φ paralleled those reported for larger colloidal spheres, showing an increase in order and a decrease in D tr by over 4 orders of magnitude. However, ligand interactions were more important near jamming, leading to different caging and jamming dynamics for smaller NPs. Finally, the normalized D tr at ultrahigh Φ depended on particle diameter and ligand molecular weight. Increasing the PEG molecular weight by a factor of 4 increased D tr by 2 orders of magnitude at ultrahigh Φ, indicating stronger ligand lubrication for smaller particles.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Analysis of a Bulk 237 Np Oxide Sample for Trace Actinides

A neptunium oxide sample was dissolved and trace actinide constituents were measured by isotope dilution ICP-MS (for 239–244 Pu, 233–238 U, 237 Np, 241–243 Am) and alpha spectrometry ( 238 Pu, 242 Cm, 244 Cm). This material contained significant quantities of transuranic elements, notably americium and curium. The isotopic composition of the material will continue to evolve over time due to radioactive decay; the measurements reported here include all isotopes decay corrected to a reference date of 1/1/2022. These factors may be considerations in criticality studies of the related 237 Np sphere.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2026

Synthesis and Reactivity of Heteroleptic U 4+ Alkyl, Benzyl, and Hydride Imidophosphorane Complexes

A series of heteroleptic U 4+ benzyl, neopentyl, and methyl complexes supported by the imidophosphorane ligand, [N = P(N,N′-ditert-butylethylenediamide)(diethylamide)] 1− (NP*), were synthesized from the monoiodide precursor, [UI(NP*) 3 ]. These heteroleptic complexes were synthesized through the selective formation of [UI(NP*) 3 ] under transmetalation conditions in the reaction between [UI 4 (1,4-dioxane) 2 ] and K[NP*]. Formation of the homoleptic complex [U(NP*) 4 ] was not observed even in the presence of excess K[NP*]. The oxidation and hydrogenolysis reactivity of the neopentyl complex, [U(Npt)- (NP*) 3 ] (Npt = neopentyl) was explored. While cyclic voltammetry indicates a potentially isolable U5+ alkyl cation, chemical oxidation of the neopentyl complex results in the isolation of a cationic U 4+ complex with a bound diethyl ether in the primary coordination sphere, [U4+(NP*)) 3 (Et 2 O)][(BArF 24 )] (BArF 24 = tetrakis(3,5-bis(trifluoromethyl)phenyl)borate). Notably, hydrogenolysis of [U(Npt)(NP*) 3 ] with H2 gas at −20 °C results in the formation of a terminal hydride intermediate confirmed by in situ NMR spectroscopy and deuterium labeling with D 2 . The connectivity and structural parameters of this hydride intermediate, [UH(NP*) 3 ], which rapidly thermally decomposes to the homoleptic complex, [U(NP*) 4 ], can be confirmed by single-crystal X-ray diffraction studies of a crystal grown by chilling the reaction mixture. The identity of [U(NP*) 4 ] was confirmed by its direct, bulk synthesis from [U(Me)(NP*) 3 ] and HNP* in a protonolysis reaction.

Alkyls↗
DOE OSTI2021

Hands-On Experimental Training [Slides]

Training provided includes: Nuclear Criticality Safety Fundamentals, Sub-Critical "Hands On" Demonstration, Hand-Stacking and Remote Approach to Critical Using the Planet Assembly, Flattop Free-Run Demonstration, and Godiva-IV Critical Assembly Demonstration.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Nuclear reactor irradiation systems and methods

A reactor irradiation method is provided that can include irradiating Np or Am spheres within a target assembly of a nuclear reactor to form reacted spheres comprising Pu. The target assembly can define a solid core within an exterior housing, and a void between the exterior housing and the solid core, wherein the spheres occupy at least a portion of the void. The irradiating can include exposing the spheres to a neutron energy spectrum while the spheres are in the void of the target assembly to form irradiated spheres.

Katalenich, Jeffrey A.↗
DOE OSTI2024

Gamma-ray imaging of Np-237 metal using an organic glass imager

Neutron and gamma-ray imaging systems are deployed within the field of nuclear safeguards for the detection and localization of special nuclear materials and other materials of interest. 237 Np is one of these materials of interest due its presence in spent nuclear fuel and potential for use in nuclear weapons when purified. Here, for the first time, a 6 kg neptunium sphere (98.8 wt% 237 Np) was measured using a dual-particle imager, from the University of Michigan, consisting of organic glass and inorganic scintillators. The novel composition of organic glass scintillator was recently developed at Sandia National Labs and has been used in particle imaging systems due to its time resolution and particle discrimination capabilities. Gamma-ray energy spectra from single and coincident events were extracted and the sequencing of Compton scatter and photoelectric absorption gamma-ray events was used to generate images using simple backprojection. The emissions of interest in this work are the 312 keV and 416 keV gamma rays from 233 Pa, a daughter isotope from the neptunium decay series. The results of this work show that there is close agreement between the true source location in angular space and the converged location from the gamma ray images created using the system. The gamma spectroscopy from single and coincident events also identified the characteristic emission from the daughter isotope and could be used to assist with the identification of 237 Np. Furthermore, successful localization of the source with 5 s of data demonstrates the practical application of the imaging system for imaging and detection of material in weapons-useable quantities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Size-Controlled Nanoparticles Embedded in a Mesoporous Architecture Leading to Efficient and Selective Hydrogenolysis of Polyolefins

A catalytic architecture, comprising a mesoporous silica shell surrounding platinum nanoparticles (NPs) supported on a solid silica sphere (mSiO2/Pt-X/SiO2; X is the mean NP diameter), catalyzes hydrogenolysis of melt-phase polyethylene (PE) into a narrow C23-centered distribution of hydrocarbons in high yield using very low Pt loadings (~10 -5 g Pt/g PE). During catalysis, a polymer chain enters a pore and contacts a Pt NP where the C–C bond cleavage occurs and then the smaller fragment exits the pore. mSiO 2 /Pt/SiO 2 resists sintering or leaching of Pt and provides high yields of liquids; however, many structural and chemical effects on catalysis are not yet resolved. Here, we report the effects of Pt NP size on activity and selectivity in PE hydrogenolysis. Time-dependent conversion and yields and a lumped kinetics model based on the competitive adsorption of long vs short chains reveal that the activity of catalytic material is highest with the smallest NPs, consistent with a structure-sensitive reaction. Remarkably, the three mSiO 2 /Pt-X/SiO 2 catalysts give equivalent selectivity. We propose that mesoscale pores in the catalytic architecture template the C 23 -centered distribution, whereas the active Pt sites influence the carbon–carbon bond cleavage rate. This conclusion provides a framework for catalyst design by separating the C–C bond cleavage activity at catalytic sites from selectivity for chain lengths of the products influenced by the structure of the catalytic architecture. The increased activity, selectivity, efficiency, and lifetime obtained using this architecture highlight the benefits of localized and confined environments for isolated catalytic particles under condensed-phase reaction conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Cocrystals combining order and correlated disorder via colloidal crystal engineering with DNA

Colloidal cocrystallization enables the formation of multicomponent materials with unique physicochemical properties, yet the role of nanoparticle (NP) shape and specific ligand interactions to cocrystallize anisotropic and isotropic NPs, with order and correlated disorder, remains underexplored. Here, geometry-inspired strategies along with programmable DNA interactions are combined to achieve structural control of colloidal cocrystal assemblies. Coassembling polyhedral and spherical NPs with complementary DNA yields two classes of cocrystals: one where both components order, and another where polyhedral NPs form a periodic lattice, while spherical NPs remain disordered but spatially correlated with polyhedral edges and corners. The size ratio of the building blocks can be used to control the ordering of spherical NPs—smaller octahedral-to-sphere size ratios favor fully ordered cocrystals. Molecular dynamics simulations further elucidate the role of NP shapes and dimensions in the structural outcome of the cocrystal. This work provides a framework for deliberately targeting and accessing crystals with exotic multicomponent structures.

Li, Yuanwei [Northwestern Univ., Evanston, IL (Uni↗
DOE OSTI2021

Exploring the kinetics of actinyl–EDTA reduction by ferrous iron using quantum-mechanical calculations

Here, the reduction of An(VI) (An = U, Np, and Pu) to An(IV) significantly decreases its solubility and mobility. This reaction can be hindered by complexation with inorganic (e.g., carbonate) or organic ligands. Ethylenediaminetetraacetic acid (EDTA) is one such organic ligand that forms stable complexes with actinides. Therefore, it may enhance the mobility of actinides. However, the redox kinetics and mechanisms of actinyl (An(V/VI)O 2 +/2+ )–EDTA are not well characterized yet and are thus studied here using quantum-mechanical calculations. The principle is to approach the actinyl–EDTA and Fe 2+ (reductant) in small incremental steps and calculate the system energy at each distance. The overall reaction is then delineated into sub-processes (encounter frequency in bulk solution, formation of outer-sphere complex, transition from outer- to inner-sphere complex, and electron transfer), and reaction rates are determined for each sub-process. The formation of outer-sphere complexes occurs rapidly in microseconds to seconds over a wide range of actinyl concentrations (pM to μM); in contrast, the transition to the inner-sphere complex is relatively slow (milliseconds to a few seconds). Immediate electron transfer to form the pentavalent actinide is observed along the reaction path for Np(VI) and Pu(VI), but not for U(VI). Surprisingly, in acidic conditions, one of the carboxylic groups gets protonated in EDTA of [UO 2 (edta)] 2- rather than one of the amino groups. This process-based series of calculations can be applied to any redox reaction and allows the prediction of changes to the rate law and rate-limiting step in a more fundamental way for different environments

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

Structural and Bonding Analysis in Monomeric Actinide(IV) Oxalate from Th(IV) to Pu(IV): Comparison with the An(IV) Nitrate Series

In this work, single-crystal X-ray diffraction (SC-XRD) structures and Raman spectra of a series of new isomorphous molecular An(IV)-oxalate compounds (Th, U, Np, and Pu) are reported. These complexes are crystallized with cobalt(III) hexamine ([Co(NH 3 ) 6 ] 3+ ) as the counter cations, [Co(NH 3 ) 6 ] 2 [An(C 2 O 4 ) 5 ]·4H 2 O, revealing five bidentate nonbridging oxalate ligands in the first coordination sphere (CN = 10). The nonbridging oxalate is rather uncommon for An(IV)-oxalate systems, which are widely characterized as polymeric compounds. Density functional theory (DFT) calculations were performed to examine the bonding between An(IV) cations and oxalate ligands. For comparison, we also report results obtained for the An(IV)-hexanitrate series, [(C 2 H 5 ) 4 N] 2 [An(NO 3 ) 6 ] (with An = Th, U, Np, Pu, and Ce), which consists of O-donor ligands as well but with a larger coordination number (CN = 12). The bonding analysis confirms that the actinide–oxygen bond is predominantly ionic with a minor increase in covalency from Th to U and slight variations from U to Pu. Further comparison showed that the charge transfer increases slightly when increasing the number of anions in the coordination sphere (C 2 O$_4^{2–}$: CN = 10; NO$_3^–$: CN = 12), but covalent effects as indicated by the amount of internuclear electron density accumulation are small and similar for oxalate and nitrate.

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

Methods of producing cobalt nanoparticles and hollow gold nanospheres and kits for practicing same

Provided are methods of producing cobalt nanoparticles (Co NPs). The methods include combining a cobalt salt, a capping agent, and a reducing agent, under Co NP synthesis conditions including a temperature selected to produce cobalt nanoparticles of a pre-selected diameter, where the temperature and pre-selected diameter are inversely related. In certain aspects, the methods further include producing hollow gold nano spheres (HGNs) using the cobalt nanoparticles as scaffolds. Also provided are cobalt nanoparticles and hollow gold nano spheres (HGNs) produced according to the present methods. Kits that find use in practicing the methods of the present disclosure are also provided.

Pu, Ying-Chih↗
DOE OSTI2022

Investigating Fission Reaction Rate Ratio Sensitivities [Abstract]

Reaction rate ratios are a measurable parameter for reactor and criticality applications. A number of foil irradiations and fission chamber measurements have been performed for critical assemblies at Los Alamos National Laboratory starting in the 1950’s including (i) Godiva, a bare HEU spherical assembly; (ii) Flattop-25, a spherical assembly consisting of an HEU core and a natural uranium reflector; (iii) Jezebel, a bare 239 Pu assembly; and (iv) Flattop-Pu, a spherical assembly consisting of a 239Pu core and a natural uranium reflector. Fission ratio data for 238 U(n,f)/ 235 U(n,f), 237 Np(n,f)/ 235 U(n,f), 233 U(n,f)/ 235 U(n,f) and 239 Pu(n,f)/ 235 U(n,f) were obtained and reported. The EUCLID (Experiments Underpinned by Computational Learning for Improvements in nuclear Data) project at Los Alamos National Laboratory (LANL) aims to constrain nuclear data by using a suite of measurement types beyond k-effective. Recent investigations include the use of pulsed spheres for nuclear data validation and other measurement methods of interest. One focus of the work is to determine if other methods are complimentary to the critical experiments utilized for nuclear data validation. It is anticipated the investigations will help inform methods that may be utilized in machine learning algorithms for nuclear validation. In order to use a measurement type for nuclear validation, it is necessary to obtain cross-section sensitivities for parameters. This work looks at reaction rate ratio sensitivities with SENSMG and Monte Carlo N-Particle R Code Version 6.21.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗