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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Low temperature hydrogen superpermeation in vanadium composite metal foil pumps

Palladium-based foil membranes are an effective option for hydrogen isotope recovery from the plasma exhaust of future fusion plants, but cost and availability are concerns. Vanadium (V) is a relatively low cost, neutron tolerant material with high hydrogen permeability. It has been well-studied as a superpermeable membrane at high temperature (>500 °C), but V displays negligible superpermeation at low temperature (75–200 °C) due to catalytic limitations. Composite membranes were fabricated by depositing thin layers (~100 nm) of either Pd or BCC PdCu on sputter-cleaned vanadium foils (100 μm). Symmetric membranes elevated superpermeation to levels approaching bulk Pd or PdCu foils, with ~5X higher flux in the latter reflecting the superior properties of PdCu. Asymmetric membranes revealed that the Pd-based catalyst layer was critical for both efficient absorption of superthermal hydrogen upstream as well as catalyzing re-combinative desorption downstream. At T ≥ 150 °C composite membrane superpermeation was equivalent to the Pd-based foils, but the flux was attenuated by a factor of 2-3X as the temperature was reduced. This deviation from pure foil performance coincided with the formation of vanadium hydride (β-V 2 H), which also impacted the transient response. Nevertheless, no embrittlement was observed under the conditions examined and elevating the temperature >150 °C removed the hydride and restored full performance. The achievement of palladium-level performance with a >99% reduction in Pd inventory makes these V composite metal foils pumps an attractive option for low temperature hydrogen isotope recovery in future fusion plants.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2017

Structure-property relationships in NO x sensor materials composed of arrays of vanadium oxide nanoclusters

Here, the mixed-valent vanadium oxide based three-dimensional framework structure species [Cd 3 (H 2 O) 12 V 16 IV V 2 V O 36 (OH) 6 (AO 4 )]∙24H 2 O, (A=V,S) (Cd 3 (VO) o ) represents a rare example of an interesting sensor material which exhibits NO x {NO+NO 2 } semiconducting gas sensor properties under ambient conditions. The electrical resistance of the sensor material Cd 3 (VO) o decreases in air. Combined characterization studies revealed that the building block, {V 18 O 42 (AO 4 )} cluster, of 3-D framework undergoes oxidation and remains intact for at least 2 months. The decrease in resistance is attributable to the reactivity of molecular oxygen towards vanadium which results in an increase in the oxidation state as well as the coordination number of vanadium center and decrease in band gap of Cd 3 (VO) o . Based on these results we propose that the changes in semiconducting properties of Cd 3 (VO) o under ambient conditions are due to the greater overlap between the O 2p and V 3d orbitals occurring during the oxidation.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Simultaneous recovery of vanadium and nickel from power plant fly-ash: Optimization of parameters using response surface methodology

Highlights: • Leaching of vanadium and nickel from fly ash (14.43% V and 5.19% Ni) in sulfuric acid was performed. • Optimization of leaching parameters was carried out using a response surface methodology. • Using optimum conditions, 94.28% V and 81.01% Ni “actual recovery” was obtained. - Abstract: Simultaneous recovery of vanadium (V) and nickel (Ni), which are classified as two of the most hazardous metal species from power plant heavy fuel fly-ash, was studied using a hydrometallurgical process consisting of acid leaching using sulfuric acid. Leaching parameters were investigated and optimized in order to maximize the recovery of both vanadium and nickel. The independent leaching parameters investigated were liquid to solid ratio (S/L) (5–12.5 wt.%), temperature (45–80 °C), sulfuric acid concentration (5–25 v/v%) and leaching time (1–5 h). Response surface methodology (RSM) was used to optimize the process parameters. The most effective parameter on the recovery of both elements was found to be temperature and the least effective was time for V and acid concentration for Ni. Based on the results, optimum condition for metals recovery (actual recovery of ca.94% for V and 81% for Ni) was determined to be solid to liquid ratio of 9.15 wt.%, temperature of 80 °C, sulfuric acid concentration of 19.47 v/v% and leaching time of 2 h. The maximum V and Ni predicted recovery of 91.34% and 80.26% was achieved.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Experimental and Theoretical Insights into the Potential of V 2 O 3 Surface Coatings for Hydrogen Permeable Vanadium Membranes

A grand challenge of vanadium-based H 2 permeable membranes is the development of effective, cheap, and stable catalysts to facilitate H 2 dissociation and recombination. This article investigates a facile air treatment to form catalytically active vanadium oxide on the surfaces of dense vanadium foils. The treatment consisted of short air exposure followed by H 2 reduction at 823 K, which produced a well-faceted and nanocrystalline V 2 O 3 layer on the foil surfaces. The resulting membranes display stable H 2 permeability of 2 ± 0.25 × 10 -8 mol·m -1 ·s -1 ·Pa -0.5 , but transient declines in permeation are observed when operated at both elevated and reduced temperatures. DFT calculations revealed that V 2 O 3 (0001) surfaces display barriers and adsorption energies for H 2 dissociation/recombination that are comparable to known H 2 activation catalysts. It was found that H 2 dissociation is expected to proceed spontaneously on metal-terminated V 2 O 3 , with recombinative-desorption anticipated as the rate limiting step.

08 HYDROGEN↗
DOE OSTI2024

Coupled Experimental–Theoretical Characterization of a Carbon Electrode in Vanadium Redox Flow Batteries using X-ray Absorption Spectroscopy

Vanadium redox flow batteries (VRFBs) have emerged as promising solutions for stationary grid energy storage due to their high efficiency, scalability, safety, near room-temperature operation conditions, and the ability to independently size power and energy capacities. The performance of VRFBs heavily relies on the redox couple reactions of V 2+ /V 3+ and VO 2+ /VO 2 + on carbon electrodes. Therefore, a thorough understanding of the surface functionality of carbon electrodes and their propensity for degradation during electrochemical cycles is crucial for designing VRFBs with extended lifespans. In this study, we present a coupled experimental–theoretical approach based on carbon K edge X-ray absorption spectroscopy (XAS) to characterize carbon electrodes prepared under different conditions and identify relevant functional groups that contribute to unique spectroscopic features. Atomic models were created to represent functional groups, such as hydroxyl, carboxyl, methyl, and aldehyde, bonded to carbon atoms in either sp 2 or sp 3 environments. The interactions between functionalized carbon and various solvated vanadium complexes were modeled using density functional theory. A library of carbon K-edge XAS spectra was generated for distinct carbon atoms in different functional groups, both before and after interacting with solvated vanadium complexes. Here we demonstrate how these simulated spectra can be used to deconvolve ex situ experimental spectra measured from carbon electrodes and to track changes in the electrode composition following immersion in different electrolytes or extended cycling within a functional VRFB. By doing so, we identify the active species present on the carbon electrodes, which play a crucial role in determining their electrochemical performance.

25 ENERGY STORAGE↗
DOE OSTI2015

Joint perpendicular anisotropy and strong interlayer exchange coupling in systems with thin vanadium spacers

We study the influence of the insertion of a vanadium spacer layer between an FeCoB layer and a [Co/Ni] multilayer in an MgO substrate-based system mimicking the reference system of a perpendicular anisotropy magnetic tunnel junction. The anisotropy of the [Co/Ni] multilayer gradually improves with the vanadium thicknesses t, up to an optimized state for t = 8 Å, with little influence of the thermal annealing. The interlayer exchange coupling is ferromagnetic and very strong for t≤6 Å. It can be adjusted by thermal treatment at t = 8 Å from no coupling in the as-grown state to more than 2 mJ/m{sup 2} after 250 °C annealing. For this spacer thickness, the magnetic properties are consistent with the occurrence of a bcc (001) to an fcc (111) crystalline structure transition at the vanadium spacer. The remaining interlayer exchange coupling at t = 8 Å is still substantially higher than the one formerly obtained with a Tantalum spacer, which holds promise for further optimization of the reference layers of tunnel junctions meant for magnetic random access memories.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Electron affinity of cubic boron nitride terminated with vanadium oxide

A thermally stable negative electron affinity (NEA) for a cubic boron nitride (c-BN) surface with vanadium-oxide-termination is achieved, and its electronic structure was analyzed with in-situ photoelectron spectroscopy. The c-BN films were prepared by electron cyclotron resonance plasma-enhanced chemical vapor deposition employing BF{sub 3} and N{sub 2} as precursors. Vanadium layers of ∼0.1 and 0.5 nm thickness were deposited on the c-BN surface in an electron beam deposition system. Oxidation of the metal layer was achieved by an oxygen plasma treatment. After 650 °C thermal annealing, the vanadium oxide on the c-BN surface was determined to be VO{sub 2}, and the surfaces were found to be thermally stable, exhibiting an NEA. In comparison, the oxygen-terminated c-BN surface, where B{sub 2}O{sub 3} was detected, showed a positive electron affinity of ∼1.2 eV. The B{sub 2}O{sub 3} evidently acts as a negatively charged layer introducing a surface dipole directed into the c-BN. Through the interaction of VO{sub 2} with the B{sub 2}O{sub 3} layer, a B-O-V layer structure would contribute a dipole between the O and V layers with the positive side facing vacuum. The lower enthalpy of formation for B{sub 2}O{sub 3} is favorable for the formation of the B-O-V layer structure, which provides a thermally stable surface dipole and an NEA surface.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Polaron-induced metal-to-insulator transition in vanadium oxides from density functional theory calculations

Vanadium oxides have been extensively studied as phase-change memory units in artificial synapses for neuromorphic computing due to their metal-insulator transitions (MIT) at or near room temperature. Recently, injection of charge carriers into vanadium oxides, e.g., via optically via a heterostructure, has been proposed as an alternative switching mechanism and also potentially as a means to tune the MIT temperature. In this study, we explore the formation of small polarons in the low temperature (LT) insulating phases for V 3 O 5 ,VO 2 , and V 2 O 3 , and the barriers to their migration using density functional theory calculations. We find that V 3 O 5 exhibits very low hole and electron polaron migration barriers (<100 meV) compared to V 2 O 3 and VO 2 , leading to much higher estimated polaronic conductivity. We also link the relative migration barriers to the amount of distortion that has to travel when the polaron migrate from one site to another. Polarons in V 3 O 5 also have smaller binding energies to vanadium and oxygen vacancy defects. Furthermore, these results suggest that the triggering of the MIT via injection of charge carriers are due to the formation of small polarons that can migrate rapidly through the crystal.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2019

High temperature deuterium enrichment using TiC coated vanadium membranes

Here, the current technology for hydrogen isotope separation requires enormous capital investment and energy consumption. Palladium-based membranes exhibit hydrogen isotope selectivity and provide a continuous method of isotope enrichment but have high material costs. Here, the authors investigate the potential of titanium carbide thin films coated on vanadium as a low-cost alternative, which enabled operation at high temperatures. Protium and deuterium exhibited nominally identical solubility in TiC coated vanadium over a range of 500–700°C. Permeation tests from 600 to 700°C revealed that protium permeated faster than deuterium, with the separation factor decreasing from 1.34 to 1.15 with increasing temperature. XPS depth-profiling showed a distinct interface between the TiC layer and the V foil in as-fabricated membranes. However, post-test analysis revealed significant V diffusion through TiC and segregation to the surface. Surface limitations resulting from this degradation accounted for changes in flux and may explain why the separation factor was lower than the value of 1.42 expected from high temperature interstitial diffusion of protium/deuterium in vanadium.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2013

Single-crystal structure of vanadium-doped La{sub 2}Mo{sub 2}O{sub 9}

A high-precision X-ray diffraction study of single crystals of two compositions-La{sub 2}Mo{sub 1.78}V{sub 0.22}O{sub 8.89} and La{sub 2}Mo{sub 1.64}V{sub 0.36}O{sub 8.82}-was performed. In the vanadium-doped compounds, as in the structure of the metastable {beta}{sub ms} phase of pure La{sub 2}Mo{sub 2}O{sub 9}, the La and Mo atoms and one of the three oxygen atoms are displaced from the threefold axis, on which they are located in the high-temperature {beta} phase. The structure contains two partially occupied oxygen sites. It was shown that molybdenum atoms are partially replaced by vanadium atoms, which are not involved in the disordering, are located on the threefold axis, and are shifted toward one of the oxygen atoms. This is consistent with the temperature-induced changes in the structure of La{sub 2}Mo{sub 2}O{sub 9} and the changes in the properties of these crystals caused by the introduction of vanadium atoms into the structure.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Switching Channel Development Dynamics in Planar Structures on the Basis of Vanadium Dioxide

The results of the experimental studies and numerical simulation of the switching channel development dynamics in planar structures on the basis of vanadium dioxide are reported. The obtained data on the variation of the temperature in the channel with time and of the current arisen after the pulsed load, and on the times of transition from the high-resistance to the low-resistance state and back are analyzed in order to determine the switching mechanism and to predict the functional characteristics of the switchable vanadium- oxide structures as promising materials for the creation of relaxation generators that can serve as prototypes of neural oscillators. It is shown that the switching behavior is associated with the metal–semiconductor phase transition in vanadium dioxide, which is stimulated by the emission of Joule heat.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Semiconductor–Metal Phase Transition and “Tristable” Electrical Switching in Nanocrystalline Vanadium Oxide Films on Silicon

Temperature dependences of the ac conductivity of nanocrystalline mixed vanadium oxide films on silicon revealed a multistep shape of the hysteresis loop observed during the semiconductor–metal phase transition in VO{sub 2}, which was not manifested in the case of dc measurements. These peculiarities are related to the size effect, heterophase character of vanadium oxide films, and different types of charge carriers in the bulk of nanocrystallites and on their surfaces. The appearance of steps is explained by the phase transition taking place in separate groups of crystallites with close dimensions. The phenomenon of “tristable” electrical switching in these vanadium oxide films was observed for the first time.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Chromium and Vanadium Incorporation in Sulfate-Containing Sodium Aluminoborosilicate Glass

In the composition space for Hanford low-activity nuclear waste glass, the waste loading of some formulations is limited by poor incorporation of sulfate. In particular, certain elements identified in previous studies tend to raise or lower sulfate solubility in borosilicate glass. The aim of the current study is to understand how vanadium and chromium each affect a sulfate-containing sodium aluminoborosilicate glass structure. Glass transition temperature, mass density, visible absorption, and Raman scattering were measured to investigate changes in the glass structure. Both Cr6+ (CrO42-) and Cr3+ were found in the chromium-containing glasses while vanadium primarily existed in the 5+ oxidation state in the vanadium-containing glasses. Electron probe microanalysis determined elemental compositions to assess retention of components. Increasing Cr2O3 caused saturation of Cr concentration within the glass and formation of crystalline eskolaite (Cr2O3). On the other hand, all the targeted V was incorporated into the glass. A fraction of batched S was not incorporated in any glass, presumably due to volatilization during melting. Apparently, the details of incorporation of Cr, and to an extent V, are different depending on whether sulfur is added as in this study or in oversaturated conditions as described in the literature, where Cr partitions to a sulfate-containing salt phase.

Borosilicate glass, Waste Glass, vanadium chemistr↗
DOE OSTI2017

Innovative coating of nanostructured vanadium carbide on the F/M cladding tube inner surface for mitigating the fuel cladding chemical interactions

Fuel cladding chemical interactions (FCCI) have been acknowledged as a critical issue in a metallic fuel/steel cladding system due to the formation of low melting intermetallic eutectic compounds between the fuel and cladding steel, resulting in reduction in cladding wall thickness as well as a formation of eutectic compounds that can initiate melting in the fuel at lower temperature. In order to mitigate FCCI, diffusion barrier coatings on the cladding inner surface have been considered. In order to generate the required coating techniques, pack cementation, electroplating, and electrophoretic deposition have been investigated. However, these methods require a high processing temperature of above 700 oC, resulting in decarburization and decomposition of the martensites in a ferritic/martensitic (F/M) cladding steel. Alternatively, organometallic chemical vapor deposition (OMCVD) can be a promising process due to its low processing temperature of below 600 oC. The aim of the project is to conduct applied and fundamental research towards the development of diffusion barrier coatings on the inner surface of F/M fuel cladding tubes. Advanced cladding steels such as T91, HT9 and NF616 have been developed and extensively studied as advanced cladding materials due to their excellent irradiation and corrosion resistance. However, the FCCI accelerated by the elevated temperature and high neutron exposure anticipated in fast reactors, can have severe detrimental effects on the cladding steels through the diffusion of Fe into fuel and lanthanides towards into the claddings. To test the functionality of developed coating layer, the diffusion couple experiments were focused on using T91 as cladding and Ce as a surrogate lanthanum fission product. By using the customized OMCVD coating equipment, thin and compact layers with a few micron between 1.5 µm and 8 µm thick and average grain size of 200 nm and 5 µm were successfully obtained at the specimen coated between 300oC and 500 oC, respectively. The coating layer contains both carbon and vanadium elements as quantified by WED, and the phases mainly consist of a mixture of V2C and VC, which was confirmed using X-ray diffraction patterns. In addition, the ratio between V and C varies with processing temperature, and it was observed that a higher temperature promotes the carbon adsorption and increases thickness of the coating. With optimized deposition conditions, we can apply the coating technique toward the actual T91 cladding materials, and provide the possibilities for the real application in sodium-cooled fast reactors (SFRs). Diffusion couple experiments were performed at both 550 oC and 690 oC, which corresponds to normal and aggressive operating temperatures, respectively. The results show that vanadium carbide coating with wider thickness (8 µm) and lower carbon concentration (27 at.%) reduced the width of the inter diffusion region, indicating that vanadium carbide coating can mitigate FCCI effectively. In specific, inter-diffusion between Fe and Ce was prohibited over most area, but Ce diffusion occurred toward the coating and the Fe substrate through thinner coating layer, which needs further optimization in terms of uniform coating thickness. Overall, it is concluded that this coating process can be successfully applied onto the inner surface of HT9 cladding tubes and the FCCI can be effectively mitigated if not totally eliminated.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Capacity Decay Mechanism of Microporous Separator-Based All-Vanadium Redox Flow Batteries and its Recovery

For all vanadium redox flow batteries (VRBs) with porous separators as membranes, convection effect is found to play a dominant role in the capacity decay of the cells over cycling by investigating the relationship between electrical performances and electrolyte compositions at both positive and negative sides. Although the concentration of total vanadium ions hardly changes at both sides over cycling, the net transfer of solutions from one side to another and thus asymmetrical valance of vanadium ions at both sides lead to the capacity fading and lower energy efficiency, which is confirmed to result from the hydraulic pressure differential at both sides of separators. In this paper, the hydraulic pressures of solutions at both sides can be in-situ monitored, and regulated by varying the gas pressures in electrolyte tanks. It is found that the capacity can be stabilized and the net transfer of solutions can be prevented by slightly tailoring the hydraulic pressure differential at both sides of separators, which, however, doesn’t work for Nafion membranes, suggesting the negligible convection factor in flow cells using Nafion membranes. Therefore, the possibility of porous separators allows long-term running for VRBs without capacity loss, highlighting a new pathway to develop membranes used in VRBs.

Li, Bin↗
DOE OSTI2022

Exploring rapid chemical separations of Sc-47 produced from photonuclear reactions on natural vanadium targets

Scandium-47 ( 47 Sc) production via bremsstrahlung irradiation of natural vanadium targets offers significant advantages for producing high purity 47 Sc; this work evaluates several rapid dissolution and chemical separation techniques for recovering high purity 47 Sc from irradiated vanadium. Here, techniques developed are combined into a simple, gram-scale, semi-automated target processing system that enables 47 Sc recovery from irradiated vanadium targets with chemical yields as high as 93 ± 3% and 47 Sc/V separation factors of 6 ± 3 ·10 11 within 90 min total processing times. Future research into H 2 O 2 resistant separation techniques and their applicability for direct process coupling to chelation are recommended.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2013

Practical thermodynamic quantities for aqueous vanadium- and iron-based flow batteries

A simple method for experimentally determining thermodynamic quantities for flow battery cell reactions is presented. Equilibrium cell potentials, temperature derivatives of cell potential (d E /d T ), Gibbs free energies, and entropies are reported here for all-vanadium, iron–vanadium, and iron–chromium flow cells with state-of-the-art solution compositions. Proof is given that formal potentials and formal temperature coefficients can be used with modified forms of the Nernst Equation to quantify the thermodynamics of flow cell reactions as a function of state-of-charge. Such empirical quantities can be used in thermo-electrochemical models of flow batteries at the cell or system level. In most cases, the thermodynamic quantities measured here are significantly different from standard values reported and used previously in the literature. The data reported here are also useful in the selection of operating temperatures for flow battery systems. Because higher temperatures correspond to lower equilibrium cell potentials for the battery chemistries studied here, it can be beneficial to charge a cell at higher temperature and discharge at lower temperature. As a result, proof-of-concept of improved voltage efficiency with the use of such non-isothermal cycling is given for the all-vanadium redox flow battery, and the effect is shown to be more pronounced at lower current densities.

25 ENERGY STORAGE↗
DOE OSTI2017

Rate mechanism of vanadium oxide coated tin dioxide nanowire electrode for lithium ion battery

Correlating composition and structures with battery performance is key aspect of electrode material design and improvement. Here utilizing in situ open cell transmission electron microscopy, we studied the in situ cycling rate performance of vanadium oxide coated tin dioxide nanowire electrode by tuning the lithiation/delithiation current. In situ results show that the good rate performance of such high capacity compositional material lies in the layered vanadium oxide coating strategy. For cycling at high rate, the layered vanadium oxide also serves as fast ions and electrons transportation route while tin nanoparticles aggregate to the surface with sizes controlled by the coating layer, cycle induced volume change is released to the surface and excellent mechanical tolerance of tin nanoparticle and inner nanowire ensure improved cyclability of the electrode.

25 ENERGY STORAGE↗