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At least 1,171 records · Page 65
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Oligomeric Ruthenium Polypyridyl Dye for Improved Stability of Aqueous Photoelectrochemical Cells

Water-splitting dye-sensitized photoelectrochemical cells rely on molecular sensitizers to harvest light energy and drive the catalytic reactions necessary to generate hydrogen and oxygen from water. The desorption of sensitizer molecules from the semiconductor–aqueous electrolyte interface is a significant barrier to the practical implementation of these cells. To address this problem, we synthesized an oligomeric ruthenium dye ([RuP] n ) that has dramatically improved stability as a photosensitizer for TiO 2 electrodes over the pH range of interest (4–7.8) for DSPECs. Additionally, the efficiency of photoelectrochemical charge separation is known to depend on the rate of cross-surface hole diffusion between dye molecules. The oligomeric dye ([RuP] n ) shows an order of magnitude faster cross-surface hole diffusion than the commonly used monomeric [Ru(bpy) 2 (4,4-PO 3 H 2 ) 2 bpy] 2+ (RuP) sensitizer. Finally, the enhanced stability of the polymeric dye also enables the use of intensity-modulated photovoltage spectroscopy to measure the recombination rate of photogenerated electrons and holes as a function of electrolyte pH.

14 SOLAR ENERGY↗
NASA NTRS1978

Numerical analyses for treating diffusion in single-, two- and three-phase binary alloy systems

Numerical solutions were applicable for planar, cylindrical, or spherical geometries with any diffusion-zone size and any continuous variation of the diffusion coefficient with concentration. Special techniques were included in the analyses to account for differences in molal volumes, initiation and growth of an intermediate phase, disappearance of a phase, and the presence of an initial composition profile in the specimen. A major improvement in solution accuracy was achieved in the two phase analysis by employing a mass conservation criterion to establish the location of the interface rather than the conventional interface-flux-balance criterion. In the three phase analysis, computation time was minimized without sacrificing solution accuracy by treating the three phase problem as a two phase problem when the thickness of the intermediate phase was less than a preset small value. Three computer codes were developed to perform these analyses.

Tenney, D. R.↗
NASA NTRS1996

Parallel Simulation of Unsteady Turbulent Flames

Time-accurate simulation of turbulent flames in high Reynolds number flows is a challenging task since both fluid dynamics and combustion must be modeled accurately. To numerically simulate this phenomenon, very large computer resources (both time and memory) are required. Although current vector supercomputers are capable of providing adequate resources for simulations of this nature, the high cost and their limited availability, makes practical use of such machines less than satisfactory. At the same time, the explicit time integration algorithms used in unsteady flow simulations often possess a very high degree of parallelism, making them very amenable to efficient implementation on large-scale parallel computers. Under these circumstances, distributed memory parallel computers offer an excellent near-term solution for greatly increased computational speed and memory, at a cost that may render the unsteady simulations of the type discussed above more feasible and affordable.This paper discusses the study of unsteady turbulent flames using a simulation algorithm that is capable of retaining high parallel efficiency on distributed memory parallel architectures. Numerical studies are carried out using large-eddy simulation (LES). In LES, the scales larger than the grid are computed using a time- and space-accurate scheme, while the unresolved small scales are modeled using eddy viscosity based subgrid models. This is acceptable for the moment/energy closure since the small scales primarily provide a dissipative mechanism for the energy transferred from the large scales. However, for combustion to occur, the species must first undergo mixing at the small scales and then come into molecular contact. Therefore, global models cannot be used. Recently, a new model for turbulent combustion was developed, in which the combustion is modeled, within the subgrid (small-scales) using a methodology that simulates the mixing and the molecular transport and the chemical kinetics within each LES grid cell. Finite-rate kinetics can be included without any closure and this approach actually provides a means to predict the turbulent rates and the turbulent flame speed. The subgrid combustion model requires resolution of the local time scales associated with small-scale mixing, molecular diffusion and chemical kinetics and, therefore, within each grid cell, a significant amount of computations must be carried out before the large-scale (LES resolved) effects are incorporated. Therefore, this approach is uniquely suited for parallel processing and has been implemented on various systems such as: Intel Paragon, IBM SP-2, Cray T3D and SGI Power Challenge (PC) using the system independent Message Passing Interface (MPI) compiler. In this paper, timing data on these machines is reported along with some characteristic results.

Menon, Suresh↗
NASA NTRS2020

The bioclimatic extent and pattern of the cold edge of the boreal forest: the circumpolar taiga-tundra ecotone

Current configurations of forest structure at the cold edge of the boreal may help understand the future of ecosystem functioning in high northern latitudes. The circumpolar biome boundary at the boreal (taiga) forest and tundra interface is an ecological transition zone (taiga-tundra ecotone; TTE) experiencing changes that affect its forest structure. We accounted for the TTE's horizontal forest structure with an estimate of its extent and pattern as represented by tree canopy cover (TCC). We quantified TCC patterns with an algorithm that describes its spatial gradient, and summarized landscape patterns of structure to represent heterogeneity, capturing abrupt, diffuse, and uniform forest at mesoscales. We used these landscape patterns to constrain the spatial extent of sparse and open canopy forest, and non-forest (forest-adjacent) edge that defines the TTE extent. The resulting map of the TTE extent is based on forest structure spatial patterns resolved at 30 m, highlights structural variability across landscapes, and helps distinguish tundra from boreal domains. We classified 14 594 landscapes as those associated with the TTE within a circumpolar bioclimatic envelope (11.575 million km2), where 44.83% of the area of these landscapes were forest and non-forest edge, yet 36.43% contributed to the TTE extent. We report the overall extent of the TTE (3.032 million km2) across North America and Greenland (53%), and Eurasia (47%), where 0.697 million km2 is non-forest edge, 0.549 million km2 is sparse forest, and 1.787 million km2 is open canopy forest. Diffuse forest landscapes dominate the TTE (79%), and abrupt landscapes (~19%) indicate portions of the TTE where sparse forest and non-forest edge are the prevailing structural patterns. This account of the TTE quantifies the area of the cold edge of the boreal forest where previous global estimates show high discrepancies, and can help target monitoring and prediction of circumpolar dynamics.

Paul M Montesano↗
DOE OSTI2020

Mesoporous nanocrystalline film architecture for capacitive storage devices

A mesoporous, nanocrystalline, metal oxide construct particularly suited for capacitive energy storage that has an architecture with short diffusion path lengths and large surface areas and a method for production are provided. Energy density is substantially increased without compromising the capacitive charge storage kinetics and electrode demonstrates long term cycling stability. Charge storage devices with electrodes using the construct can use three different charge storage mechanisms immersed in an electrolyte: (1) cations can be stored in a thin double layer at the electrode/electrolyte interface (non-faradaic mechanism); (2) cations can interact with the bulk of an electroactive material which then undergoes a redox reaction or phase change, as in conventional batteries (faradaic mechanism); or (3) cations can electrochemically adsorb onto the surface of a material through charge transfer processes (faradaic mechanism).

25 ENERGY STORAGE↗
DOE OSTI2024

Mesoporous nanocrystalline film architecture for capacitive storage devices

A mesoporous, nanocrystalline, metal oxide construct particularly suited for capacitive energy storage that has an architecture with short diffusion path lengths and large surface areas and a method for production are provided. Energy density is substantially increased without compromising the capacitive charge storage kinetics and electrode demonstrates long term cycling stability. Charge storage devices with electrodes using the construct can use three different charge storage mechanisms immersed in an electrolyte: (1) cations can be stored in a thin double layer at the electrode/electrolyte interface (non-faradaic mechanism); (2) cations can interact with the bulk of an electroactive material which then undergoes a redox reaction or phase change, as in conventional batteries (faradaic mechanism); or (3) cations can electrochemically adsorb onto the surface of a material through charge transfer processes (faradaic mechanism).

Dunn, Bruce S.↗
DOE OSTI2023

Reducing ion diffusion at atmospheric pressure through intermingled positive and negative ions

Increasing ion molecule reaction times for ambient ionization techniques can increase sensitivity of detection. Longer reaction times result in an increase in analyte signal relative to the reactant ion signal, however with a subsequent decrease in the total ion intensity. This loss in the total number of ions reaching the detector limits the extent to which increased reaction time can improve detection in practical applications. In this study ion loss was measured using either electric fields or gas flow to control ion transit time. Ion transit times ranged from 40 ms to 8s, which resulted in ion densities ranging from 5 x 10 6 to 2 x 10 4 ions/cm 3 , respectively. These results provide insights into practical reaction time limitations or experimental boundaries when exploring sensitivity enhancements in ambient ionization. When exploring longer reaction times with an atmospheric flow tube coupled to a mass spectrometer (AFT-MS), an additional corona discharge ionization source of the same polarity was added in an attempt to increase total ion signal, but no improvement in signal was observed. This observation suggested that there was a maximum ion density being reached by the corona discharge that could not be increased by adding more of the same polarity ions. A hypothesis was that intermingling both polarities of ions would reduce ion loss and increase the measured ion signal. When two corona discharge sources—one each of positive and negative polarity—were used simultaneously in an AFT-MS, the total ion signal of either polarity measured by the MS was approximately double the current from a single corona discharge source. An increase in the negative ion signal was also observed when ~10 parts-per-trillion vapor levels of an explosive (RDX) were introduced. In this case both the nitrate reactant ions and the RDX signal more than doubled with the addition of a corona discharge source producing positive ions. When intermingling positive and negative ions, an increase in ion current was also observed when the AFT was coupled directly to a Faraday detector or to an ion mobility spectrometer. This was the first demonstration of interfacing the AFT to an IMS. The observations and developments from this work will help in creating more portable instruments with improved sensitivity for detection of chemicals.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

In Situ Investigation of Chemomechanical Effects in Thiophosphate Solid Electrolytes

Solid-state batteries can suffer from catastrophic failure at high current densities due to solid electrolyte fracture, interface decomposition, or lithium filament growth. Failure is linked to chemomechanical material transformations that can manifest during electrochemical cycling. We systematically investigate how solid electrolyte microstructure and interfacial decomposition (e.g., interphase) affect failure mechanisms in lithium thiophosphates (Li3PS4, LPS) electrolytes. Kinetically metastable interphases are engineered with iodine doping, and microstructural control is achieved using milling and annealing processing techniques. In situ transmission electron microscopy reveals iodine diffusion to the interphase, and upon electrochemical cycling, pores are formed in the interphase region. In situ synchrotron tomography reveals that interphase pore formation drives edge fracture events, which are the origin of through-plane fracture failure. Fractures in thiophosphate electrolytes actively grow toward regions of higher porosity and are affected by heterogeneity in microstructure (e.g., porosity factor). This report provides fundamental design guidelines for high-performance solid-state batteries.

25 ENERGY STORAGE↗
DOE OSTI2022

Thermal model for time-domain thermoreflectance experiments in a laser-flash geometry

Time-domain thermoreflectance (TDTR) is a well-established pump–probe method for measuring thermal conductivity and interface conductance of multilayers. Interpreting signals in a TDTR experiment requires a thermal model. In standard front/front TDTR experiments, both pump and probe beams typically irradiate the surface of a multilayer. As a result, existing thermal models for interpreting thermoreflectance experiments assume that the pump and probe beams both interact with the surface layer. Here, we present a frequency-domain solution to the heat-diffusion equation of a multilayer in response to nonhomogeneous laser heating. This model allows analysis of experiments where the pump and probe beams irradiate opposite sides of a multilayer. We call such a geometry a front/back experiment to differentiate such experiments from standard TDTR experiments. As an example, we consider a 60nm amorphous Si film. We consider how signals differ in a front/front vs front/back geometry and compare thermal model predictions to experimental data.

Peng, Wanyue↗
NASA NTRS1973

Application of diffusion bonding to electronic interconnection of flatpack leads

Diffusion-bonded joints between gold-plated Kovar leads and indium-plated copper circuit pads offer some advantages for electronic circuit packaging. Test results show that consistent high strength bonds stronger than the copper circuit foil are achieved by parallel-gap bonding at relatively low power settings. The bonds are basically formed by the alloying of the gold, indium and copper at the bond interface. Other low melting metals such as tin can also be used; however, tin does not offer the ease of bonding that results in consistent separation of the copper foil during pull testing. The investigation was conducted in three parts consisting of: (1) an evaluation of the physical strength of resulting bonds at ambient and elevated temperature, (2) a metallurgical analysis of bonds using scanning electron microscopy and nondispersive X-ray analysis, and (3) evaluation and development of various schemes for multiple lead flatpack bonding.

Korb, R. W.↗
NASA NTRS1993

Mixing and unmixedness in plasma jets 1: Near-field analysis

The flow characteristics in the near-field of a plasma jet are simulated with a two-fluid model. This model accounts for both gradient-diffusion mixing and uni-directional sifting motion resulting from pressure-gradient-body-force imbalance. This latter mechanism is believed to be responsible for the umixedness observed in plasma jets. The unmixedness is considered to be essentially a Rayleigh-Taylor kind instability. Transport equations are solved for the individual plasma and ambient gas velocities, temperatures and volume fractions. Empirical relations are employed for the interface transfers of mass, momentum and heat. The empirical coefficients are first established by comparison of predictions with available experimental data for shear flows. The model is then applied to an Argon plasma jet ejecting into stagnant air. The predicted results show the significant build-up of unmixed air within the plasma gas, even relatively far downstream of the torch. By adjusting the inlet condition, the model adequately reproduces the experimental data.

Ilegbusi, Olusegun J.↗
NASA NTRS2006

Global Energy and Aviation Concerns

Renewable energy sources are usually diffuse and require large facilities. Biofuels work better, are more economical to produce for ground transportation, but sharply increase competition for food croplands. Noble laureate Richard Smalley (deceased-2005) conceptual 20 TWe power generation covers hundreds x hundreds of miles. Combined with Fuller s superconducting power grid system would enable renewable planetary energy. A solar-wind project in Australia will have a 7km diameter collector interfacing with a 1 km tower to extract 200 MW from wind turbines mounted at the base. GE Energy s 3.5MW Wind Turbine is large and placing this in perspective, it is as if one were rotating a Boeing 747-200; the blade diameter is that large. Wind turbines are rapidly gaining popularity in Europe and photovoltaic (PV) is expected to also expand rapidly. It becomes clear that we need (and still have time) to develop new sources of energy. Hf 178 bombarded by X-rays produces Gamma-rays for heating. The reaction stops when the X-rays stop; the half life is about 30 years and seems manageable vs 30 000 years. Water splitting needs to be perused as do ultra fast ultra intense laser applications in terms of fusion and new materials developments including new ways to strip and re-bind hydrogen into fuels. New methods and tools for development are being found in quantum mechanical applications to macro-systems and need to be developed into a set of new tool boxes for development of these new energy sources.

Hendricks, Robert C.↗
NASA NTRS2005

Video Mosaicking for Inspection of Gas Pipelines

A vision system that includes a specially designed video camera and an image-data-processing computer is under development as a prototype of robotic systems for visual inspection of the interior surfaces of pipes and especially of gas pipelines. The system is capable of providing both forward views and mosaicked radial views that can be displayed in real time or after inspection. To avoid the complexities associated with moving parts and to provide simultaneous forward and radial views, the video camera is equipped with a wide-angle (>165 ) fish-eye lens aimed along the axis of a pipe to be inspected. Nine white-light-emitting diodes (LEDs) placed just outside the field of view of the lens (see Figure 1) provide ample diffuse illumination for a high-contrast image of the interior pipe wall. The video camera contains a 2/3-in. (1.7-cm) charge-coupled-device (CCD) photodetector array and functions according to the National Television Standards Committee (NTSC) standard. The video output of the camera is sent to an off-the-shelf video capture board (frame grabber) by use of a peripheral component interconnect (PCI) interface in the computer, which is of the 400-MHz, Pentium II (or equivalent) class. Prior video-mosaicking techniques are applicable to narrow-field-of-view (low-distortion) images of evenly illuminated, relatively flat surfaces viewed along approximately perpendicular lines by cameras that do not rotate and that move approximately parallel to the viewed surfaces. One such technique for real-time creation of mosaic images of the ocean floor involves the use of visual correspondences based on area correlation, during both the acquisition of separate images of adjacent areas and the consolidation (equivalently, integration) of the separate images into a mosaic image, in order to insure that there are no gaps in the mosaic image. The data-processing technique used for mosaicking in the present system also involves area correlation, but with several notable differences: Because the wide-angle lens introduces considerable distortion, the image data must be processed to effectively unwarp the images (see Figure 2). The computer executes special software that includes an unwarping algorithm that takes explicit account of the cylindrical pipe geometry. To reduce the processing time needed for unwarping, parameters of the geometric mapping between the circular view of a fisheye lens and pipe wall are determined in advance from calibration images and compiled into an electronic lookup table. The software incorporates the assumption that the optical axis of the camera is parallel (rather than perpendicular) to the direction of motion of the camera. The software also compensates for the decrease in illumination with distance from the ring of LEDs.

Magruder, Darby↗
DOE OSTI2025

Binding and Translocation of Substrate Allosterically Promotes Functional Interactions Within the AlkB–AlkG Electron Transfer Complex

The alkane monooxygenase AlkB and rubredoxin AlkG form an electron transfer complex that hydroxylates terminal alkanes to produce alcohols. The recent cryoEM study of Fontimonas thermophila AlkB-AlkG complex revealed its architecture, including a dodecane (D12) substrate at the active site. However, FtAlkBG molecular mechanism of action of remains unknown. Here, in this study, we examined its dynamics and interactions by multiscale computations, including molecular dynamics simulations, elastic network models, and QM/MM of the oxygen activation mechanism at the AlkB catalytic site. D12 maintained stable interactions within the catalytic site during two MD runs, coordinated by hydrophobic residues L263-L264, I267, I133. A third extended run revealed that D12 could translocate to a membrane-exposed site near S49/F46 along a hydrophobic channel gated by I54. During this translocation, D12 was temporarily stabilized at intermediate sites IS1 (lined by I27/L30-G31/G50/L53-I54/P59/S124/A127-V128) and IS2 (I33-G34/L37/L45-F46/S49) before nearly exiting the protein, and diffused back to the active site, assisted by L30. Substrate binding and translocation across those intermediate sites affects the coupling between the iron centers in AlkBG, and interfacial interactions between AlkB-AlkG. The channel was further connected to the cytosol, near two surface-exposed arginines, potentially allowing for O 2 passage. The allosteric effects between D12 putative entry site, catalytic site and AlkB-AlkG interface were analyzed by ENM-based methods which confirmed the cooperative perturbation-responses and strongly correlated movements of residues belonging to those distal regions. Our study provides new mechanistic insights into key sites and their interactions that could be targeted for developing AlkB-variants with desirable alkane conversion functions.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Fuel-cladding chemical interaction of a prototype annular U-10Zr fuel with Fe-12Cr ferritic/martensitic HT-9 cladding

As an alternative fuel form, the annular metallic fuel design eliminates the liquid sodium bond between the fuel and the cladding, providing back-end fuel cycle and other benefits. The fuel-cladding chemical interaction (FCCI) of annular fuel also presents new features. In this work, state-of-the-art electron microscopy and spectroscopy techniques were used to study the FCCI of a prototype annular U-10wt%Zr (U-10Zr) fuel with ferritic/martensitic HT-9 cladding irradiated to 3.3% fission per initial heavy atom. Compared with sodium-bonded solid fuels, negligible amounts of lanthanides were found in the FCCI layer in the investigated helium-bonded annular fuel. Instead, most lanthanides were retained in the newly formed UZr 2 phase in the fuel center region. The interdiffusion of iron and uranium resulted in tetragonal ( U ,Zr) 6 Fe phase (space group I4/mcm) and cubic ( U ,Zr)( Fe ,Cr) 2 phase (space group Fd 3 ¯ m). The ( U ,Zr)( Fe ,Cr) 2 phase contains a high density of voids and intergranular uranium monocarbides of NaCl-type crystal structure (space group Fm 3 ¯ m). At the interdiffusion zone and inner cladding interface, a porous lamellar structure composed of alternating Cr-rich layers and U-rich layers was observed. Next to the lamellar region, the unexpected phase transformation from body-centered cubic ferrite (α-Fe) to tetragonal binary Fe-Cr σ phase (space group P4 2 /mnm) occurred, and tetragonal Fe-Cr-U-Si phase (space group I4/mmm) was identified. Due to the diffusion of carbon into the interdiffusion zone, carbon depletion inside the HT-9 led to the disappearance of the martensite lath structure, and intergranular U-rich carbides formed as a result of the diffusion of uranium into the cladding. These detailed new findings reveal the unique features of the FCCI behavior of annular U-Zr fuels, which could be a promising alternative fuel form for high burnup fast reactor applications.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Adhesively Bonded Copper and Polyimide for Flexible Printed Circuit Boards: A Data-Driven Degradation Study Under Accelerated Aging

The long-term durability of polyimide laminated adhesive based flexible printed circuit boards (PCBs) is critical to the microelectronics industry. The interface of the adhesive layer binding the polyimide and copper layers is particularly vulnerable since decreased bonding strength can lead to deadhesion, performance loss, and premature device failure. Here, in this study, adhesive-bonded polyimide and copper samples are subjected to 1000 h of damp heat exposure (85 °C/85%RH) to evaluate the impact of moisture and copper inclusion on the adhesive bonding performance. Significant copper diffusion through the adhesive layer is observed, which, combined with moisture uptake, is found to substantially weaken interfacial adhesion in copper-containing samples, thereby reducing device lifetime. Observed surface and bulk material changes are correlated to adhesion strength using the network structural equation modeling (netSEM) approach, resulting in a robust predictive model of performance degradation based on measurable materials properties.

Chemistry↗
DOE OSTI2024

Pore‐Scale Modeling of Reactive Transport with Coupled Mineral Dissolution and Precipitation

Abstract We present a new pore‐scale model for multicomponent advective‐diffusive transport with coupled mineral dissolution and precipitation. Both dissolution and precipitation are captured simultaneously by introducing a phase transformation vector field representing the direction and magnitude of the overall phase change. An effective viscosity model is adopted in simulating fluid flow during mineral dissolution‐precipitation that can accurately capture the velocity field without introducing any empirical parameters. The proposed approach is validated against analytical solutions and interface tracking simulations in simplified structures. After validation, the proposed approach is employed in modeling realistic rocks where mineral dissolution and precipitation are dominant at different locations. We have identified three regimes for mineral dissolution‐precipitation coupling: (a) compact dissolution‐precipitation where dissolution is dominant near the inlet and precipitation is dominant near the outlet, (b) wormhole dissolution with clustered precipitation where dissolution generates wormholes in the main flow paths and precipitation clogs the secondary flow paths, and (c) dissolution dominant where all solid grains are gradually dissolved. In the three regimes, the proposed approach provides reliable porosity‐permeability relationships that cannot be described well by traditional macroscale models. We find that the permeability can increase while the overall porosity decreases when the main flow paths are expanded by dissolution and adjacent pore spaces are clogged by precipitation.

58 GEOSCIENCES↗
DOE OSTI2020

Bipolar membrane polarization behavior with systematically varied interfacial areas in the junction region

The palette of applications for bipolar membranes (BPMs) has expanded recently beyond electrodialysis as they are now being considered for fuel cell and electrolysis applications. Their deployment in emerging electrochemical technologies arises from the need to have a membrane separator that provides disparate pH environments and to prevent species crossover. Most materials research for BPMs has focused on water dissociation catalysts and less emphasis has been given to the design of the polycation–polyanion interface for improving BPM performance. Here, soft lithography fabricated a series of micropatterned BPMs with precise control over the interfacial area in the bipolar junction. Polarization experiments showed that a 2.28× increase in interfacial area led to a 250 mV reduction in the onset potential. Additionally, the same increase in interfacial area yielded marginal improvements in current density due to the junction region being under kinetics-diffusion control. A simple physics model based on the electric field of the junction region rationalized the reduction in the overpotential for water dissociation as a function of interfacial area. Finally, the soft lithography approach was also conducive for fabricating BPMs with different chemistries ranging from perfluorinated polymer backbones to alkaline stable poly(arylene) hydrocarbon polymers. These polymer chemistries are better suited for fuel cell and electrolysis applications. The BPM featuring the alkaline stable poly(terphenyl) anion exchange membrane had an onset potential of 0.84 V, which was near the thermodynamic limit, and was about 150 mV lower than a commercially available variant.

25 ENERGY STORAGE↗