Stabilization of a nanoporous NiCu dilute alloy catalyst for non-oxidative ethanol dehydrogenation
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99 GENERAL AND MISCELLANEOUS↗
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Single-state selection system for hydrogen masers
The design and operation of a single-state selection system based on the adiabatic fast-passage technique for atomic state inversion is described. The system uses a variable-pitch dc solenoid and orthogonal four-wire RF coil to create the state-changing magnetic fields, and a half-wavelength state selection magnet to remove the inverted state atoms from the hydrogen beam. The system's performance was determined by measuring maser power as a function of line Q. The system removes more than 85 percent of undesired atoms from the beam. The potential effects of improvements in the maser on its frequency stability have been calculated. The use of single-state selection combined with increased RF coupling to the cavity and increased storage bulb collimation offers the possibility of frequency stability in the 10 to the -17th regime over intervals on the order of 60,000 s.
Mattison, Edward M.↗
Determining the Role of Synthesis and Reaction Conditions on the Exposed Surface and Shape of ..beta..-Mo2C Catalysts
The production of drop-in quality biofuels typically can be achieved through catalytic fast pyrolysis (CFP) of biomass, followed by hydrodeoxygenation (HDO) of the vapor-phase product to reduce the oxygen content and stabilize the bio-oil product. To favor selectivity toward desired deoxygenation products, bifunctional catalysts with both acidic and hydrogenation sites are often employed. Due to both its oxophilicity and its ability to promote hydrogenation reactions, molybdenum carbide catalysts have shown promise for promoting the HDO of CFP vapors. However, the surface structure and composition of carbide catalyst particles are not well understood, precluding the establishment of fundamental structure-function relationships needed for the rational development of molybdedum carbide for HDO, as well as other reactions. For orthorhombic ..beta..-Mo2C, the (100) facet is largely studied for computational surface-reaction analyses, possibly due to its similarities with the close-packed (111) facet of noble-metal catalysts. However, it has previously been postulated through ab initio thermodynamic studies that the (111), (110), and (011) facets are most stable, though there is no consensus. Furthermore, while a majority of previous surface stability analyses of ..beta..-Mo2C focus on bulk terminations, the highly carburizing synthesis conditions and the use of ..beta..-Mo2C in carbon-containing reaction applications could introduce non-stoichiometric coverages of surface carbon. As such, this study uses ab initio thermodynamics calculations to assess the relative surface stability of the low-index facets of ..beta..-Mo2C, including consideration of varying the coverage of surface carbon. From this information, Wulff constructions are utilized to predict the synthesis and reaction condition-dependent shape and surface carbon composition of ..beta..-Mo2C catalyst particles.
BIOMASS FUELS,INORGANIC, ORGANIC, PHYSICAL, AND AN↗
Fundamental Science for Enhancing the Durability of Photoelectrodes for Solar Fuels Production
During the award period, we performed a series of investigations to address a key bottleneck in solar-driven fuel production, which is materials stability. Regardless of the activity of electrocatalysts or selectivity of products, or efficiency of the light absorbers, if the systems are not stable then there is no ultimate technological relevance for solar fuels production. Degradation of semiconductor photoelectrodes is a well-known, long-recognized impediment to implementation of practical stable solar fuels systems. Thus, we aimed to define the thermodynamics and kinetics of the (electro)chemical processes that underpin corrosion of semiconductor photoelectrodes. We also sought to develop protective coatings and kinetic control strategies to extend durability of semiconductor photoelectrodes.
14 SOLAR ENERGY↗
Assessment of Terra MODIS Thermal Emissive Band Calibration Using Cold Targets and Measurements in Lunar Roll Events
Terra MODIS has provided continuous global observations for science research and applications for more than 18 years. The MODIS Thermal emissive bands (TEB) radiometric calibration uses a quadratic function for instrument response. The calibration coefficients are updated using the response of an on-board blackbody (BB) in quarterly warm-up and cool-down (WUCD) events. As instrument degradation and electronic crosstalk of long-wave infrared (LWIR) bands 27 to 30 developed substantial issues, accurate calibration is crucial for a high-quality L1B product. The on-board BB WUCD temperature ranges from 270 K to 315 K and the derived nonlinear response has a relatively large uncertainty for the offset, especially for these LWIR bands, which affects the measurements of low brightness temperature (BT) scenes. In this study, the TEB radiometric calibration impact on the L1B product is assessed using selected cold targets and the measurements during regular lunar rolls. The cold targets include Antarctic Dome Concordia (Dome-C) and deep convective clouds (DCC) for the calibration assessment, focusing on bands 27 to 30. Dome-C area is covered with uniformly-distributed permanent snow, and the atmospheric effect is small and relatively constant. Usually the DCC is treated as an invariant earth target to evaluate the reflective solar band calibration. The DCC can also be treated as a stable target to assess the performance of TEB calibration. During a scheduled lunar observation event with a spacecraft roll maneuver to view the moon through the space view port, the instrument cavity provides a stable reference for calibration assessment. The long-term trending of BT measurements and the relative difference between scan mirror sides and detectors are used for the assessment of the calibration consistency and stability. The comparison of L1B products over the selected targets before and after the calibration coefficients update can be used to assess the impact of a calibration look-up table (LUT) update. This assessment is beneficial for future calibration algorithm and LUT update procedure improvements for enhancing the L1B product quality.
Chang, Tiejun↗
Composition-dependent stability of the medium-range order responsible for metallic glass formation
The competition between the characteristic medium-range order corresponding to amorphous alloys and that in ordered crystalline phases is central to phase selection and morphology evolution under various processing conditions. We examine the stability of a model glass system, Cu–Zr, by comparing the energetics of various medium-range structural motifs over a wide range of compositions using first-principles calculations. Furthermore, we focus specifically on motifs that represent possible building blocks for competing glassy and crystalline phases, and we employ a genetic algorithm to efficiently identify the energetically favored decorations of each motif for specific compositions. These results show that a Bergman-type motif with crystallization-resisting icosahedral symmetry is energetically most favorable in the composition range 0.63 < xCu < 0.68, and is the underlying motif for one of the three optimal glass-forming ranges observed experimentally for this binary system (Li et al., 2008). This work establishes an energy-based methodology to evaluate specific medium-range structural motifs which compete with stable crystalline nuclei in deeply undercooled liquids.
36 MATERIALS SCIENCE↗
Investigations of the potential performance characteristics of selected contact lubricants for applications in miniature slip-ring capsules of the type used in ST 124 M stabilized inertial guidance platforms Final technical report, 27 Mar. 1968 - 30 Apr. 1970
Performance characteristics of liquid and solid lubricants for contacts of miniature slip-ring capsules
Baker, J. B.↗
Effect of fiber reinforcement on thermo-oxidative stability and mechanical properties of polymer matrix composites
A number of studies have investigated the thermooxidative behavior of polymer matrix composites. Two significant observations have been made from these research efforts: (1) fiber reinforcement has a significant effect on composite thermal stability; and (2) geometric effects must be considered when evaluating thermal aging data. The polyimide PMR-15 was the matrix material used in these studies. The control composite material was reinforced with Celion 6000 graphite fiber. T-4OR graphite fibers, along with some very stable ceramic fibers were selected as reinforcing fibers because of their high thermal stability. The ceramic fibers were Nicalon (silicon carbide) and Nextel 312 (alumina-silica-boron oxide). The mechanical properties of the two graphite fiber composites were significantly different, probably owing to variations in interfacial bonding between the fibers and the polyimide matrix. Three oxidation mechanisms were observed: (1) the preferential oxidation of the Celion 6000 fiber ends at cut surfaces, leaving a surface of matrix material with holes where the fiber ends were originally situated; (2) preferential oxidation of the composite matrix; and (3) interfacial degradation by oxidation. The latter two mechanisms were also observed on fiber end cut surfaces. The fiber and interface attacks appeared to initiate interfiber cracking along these surfaces.
Bowles, K. J.↗
High Resolution X-Ray Explorer (HIREX)
SAO is involved in a study to determine the feasibility of building an orbiting telescope capable of resolving 7 km structure on the Sun. In order to achieve the required imaging the telescope must have a resolution 0.01 arcsec. This fact challenges the state of the art of orbiting telescopes in several areas: Mirror Figuring; Optical Metrology; Optical Mounting; Mirror Figure Control; System Alignment; Optical Stability; Observatory Pointing; and Image Stability. The telescope design concept is based on a 0.6 m Gregorian-style telescope with a 240 meter effective focal length. This is achieved with 2 mirrors supported at opposite ends of a 35 m space-deployable boom. The telescope mirrors are coated with multilayers designed to reflect a broad XUV passband. A third, small mirror, near the focal plane performs the function of selecting the narrow band that is finally imaged. Image stabilization to the 0.005 arcsec level is achieved by active control of the secondary mirror. The primary mirror is held unadjustably to the spacecraft, its pointing set by the spacecraft orientation. The secondary mirror is mounted on a 6-axis stage that permits its position to be changed to align the telescope in space. The stage is intended for intermittent adjustment, both because of its speed of travel, and the TBD alignment procedure. The third mirror is called the TXI (Tuneable X-ray Imager). It is mounted on a gimbal that permits it to be tipped over a 60 degree range, selecting between the individual wavelengths in the initial bandpass. It can also rotated completely out of the way to allow the full, broadband EUV flux to strike the focal plane. Finally, the focal plane assembly is designed to rotate on the outer edge of a circle centered on the TXI mirror rotation axis. This permits the focal plane to move to the location that the TXI redirects the light once it has been set to a given wavelength response. The Engineering Study is divided into the following areas: Mirror Fabrication and Metrology; Optical Layout-Trade Study between On-axis and Off-axis; Overall System Design; and Pointing Control/Image Stabilization. The observational goals of the mission are described in the Mission Requirements document. The work is being performed to the requirements called out in the Science Requirements document.
Goulb, Leon↗
Design of super-strong and thermally stable nanotwinned Al alloys via solute synergy
Al alloys have widespread industrial applications. However, their mechanical strength is often much lower than steels. Here, we investigate the influence of solutes on achieving ultrahigh strength and thermal stability of nanotwinned Al alloys. In situ micropillar compression tests show the addition of a small amount of Ti can significantly increase the mechanical strength of Al–Ni alloys to 2 GPa. Deformation induced detwinning, Ni segregation and grain coarsening as discovered in binary Al–Ni alloys are mostly absent in the ternary Al–Ni–Ti alloys. Moreover, the ternary Al–Ni–Ti alloys have outstanding thermal stability. Density function theory calculations reveal the synergetic pinning effect of Ni–Ti solute pairs on incoherent twin boundaries. This study demonstrates that the proper selection of synergistic solute pairs is critical to improve the thermal stability and mechanical properties of nanotwinned Al alloys.
36 MATERIALS SCIENCE↗
Effect of Ni content on the morphological evolution of Ni-YSZ solid oxide fuel cell electrodes
The coarsening of Ni in Ni–yttria-stabilized zirconia (YSZ) anodes is a potential cause of long term solid oxide fuel cells (SOFC) performance degradation. The specifics of the Ni-YSZ structure—including Ni/YSZ ratio, porosity, and particle size distributions—are normally selected to minimize anode polarization resistance, but they also impact long-term stability. A better understanding of how these factors influence long-term stability is important for designing more durable anodes. The effect of structural details, e.g., Ni-YSZ ratio, on Ni coarsening has not been quantified. Furthermore, prior measurements have been done by comparing evolved structures with control samples, such that sample-to-sample variations introduce errors. Here in this paper, we report a four dimensional (three spatial dimensions and time) study of Ni coarsening in Ni-YSZ anode functional layers with different Ni/YSZ ratios, using synchrotron x-ray nano-tomography. The continuous structural evolution was observed and analyzed at sub-100 nm resolution. It is shown quantitatively that increasing the Ni/YSZ ratio increases the Ni coarsening rate. This is due to both increased pore volume and a decrease in the YSZ volume fraction, such that there is more free volume and a less obtrusive YSZ network, both of which allow greater Ni coarsening. The results are shown to be in good agreement with a power-law coarsening model. In conclusion, the finding is critical for informing the design of SOFC electrode microstructures that limit coarsening and performance degradation.
36 MATERIALS SCIENCE↗
Copper-Doped Tin Oxides Supported on Mesoporous Carbon Xerogel for Boosting the Electrochemical Reduction of CO 2 to Formate in Bicarbonate Solution Coupled with CO 2
The electrochemical reduction of CO 2 into valuable products at mild reaction conditions and using cheap renewable electrical energy are goals to sustain a low-carbon economy. Among the various CO 2 reduction reaction products, formic acid (FA) has received significant attention because of its low Gibbs free energy input requirement and the simple reduction reaction involving the transfer of 2 electrons and 2 protons. In this work, a copper-doped tin oxide catalyst supported on a mesoporous carbon xerogel was shown to enhance the electrochemical reduction of CO 2 to formate in a bicarbonate solution coupled with CO 2 . We observed that the synergistic SnCu oxides enhance the selectivity toward formate from 58.6% for Sn oxide and 28.7% for Cu oxide to over 71.2% for the SnCu oxides. The observed rate of formate production with SnCu oxide was 2.8 times higher compared to the rate of Cu oxide and about 1.5 times higher than with the Sn oxide catalyst. Our results reveal that selectivity for formate comes partly from the electrolysis of the bicarbonate solution and partly from continuous CO 2 gas purged into the solution. The contribution from the electrolysis of bicarbonate solution ranges from 15% to 40% when the concentration of bicarbonate solution ranges from 100 mM to 1 M. Chronoamperometric measurements for stability revealed that Cu oxide and Sn oxide showed stable current density for less than 30 h while under the same conditions, the stable current density was observed for more than 50 h with SnCu oxide catalyst. Additionally, the selectivity toward formate increased by 6% when the reactor pressure was increased from near ambient pressure to 4 psig. Our lab-scale electrochemical cell with SnCu oxide supported on the mesoporous carbon xerogel enhances the CO 2 solubility, minimizes the precipitation of salts that can degrade the catalytic performance, and suppresses the competitive hydrogen evolution reaction, demonstrating the feasibility of using our catalyst and system for the electrochemical conversion of CO 2 into formate with high selectivity, productivity, and stability. Furthermore, this could have significant implications for the mitigation of CO 2 emissions and the development of a sustainable chemical industry.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
On the stability and compressive nonlinearity of a physiologically based model of the cochlea
Hearing relies on a series of coupled electrical, acoustical (fluidic) and mechanical interactions inside the cochlea that enable sound processing. A positive feedback mechanism within the cochlea, called the cochlear amplifier, provides amplitude and frequency selectivity in the mammalian auditory system. The cochlear amplifier and stability are studied using a nonlinear, micromechanical model of the Organ of Corti (OoC) coupled to the electrical potentials in the cochlear ducts. It is observed that the mechano-electrical transduction (MET) sensitivity and somatic motility of the outer hair cell (OHC), control the cochlear stability. Increasing MET sensitivity beyond a critical value, while electromechanical coupling coefficient is within a specific range, causes instability. We show that instability in this model is generated through a supercritical Hopf bifurcation. A reduced order model of the system is approximated and it is shown that the tectorial membrane (TM) transverse mode effect on the dynamics is significant while the radial mode can be simplified from the equations. The cochlear amplifier in this model exhibits good agreement with the experimental data. A comprehensive 3-dimensional model based on the cross sectional model is simulated and the results are compared. It is indicated that the global model qualitatively inherits some characteristics of the local model, but the longitudinal coupling along the cochlea shifts the stability boundary (i.e., Hopf bifurcation point) and enhances stability.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Expanding the application of a UV-visible reporter for transient gene expression and stable transformation in plants
Abstract Green fluorescent protein (GFP) has been widely used for monitoring gene expression and protein localization in diverse organisms. However, highly sensitive imaging equipment, like fluorescence microscope, is usually required for the visualization of GFP, limitings its application to fixed locations in samples. A reporter that can be visualized in real-time regardless the shape, size and location of the target samples will increase the flexibility and efficiency of research work. Here, we report the application of a GFP-like protein, called eYGFPuv, in both transient expression and stable transformation, in two herbaceous plant species ( Arabidopsis and tobacco) and two woody plant species (poplar and citrus). We observed bright fluorescence under UV light in all of the four plant species without any effects on plant growth or development. eYGFPuv was shown to be effective for imaging transient expression in leaf and root tissues. With a focus on in vitro transformation, we demonstrated that the transgenic events expressing 1x eYGFPuv could be easily identified visually during the callus stage and the shoot stage, enabling early and efficient selection of transformants. Furthermore, whole-plant level visualization of eYGFPuv revealed its ubiquitous stability in transgenic plants. In addition, our transformation experiments showed that eYGFPuv can also be used to select transgenic plants without antibiotics. This work demonstrates the feasibility of utilizing 1x eYGFPuv in studies of gene expression and plant transformation in diverse plants.
59 BASIC BIOLOGICAL SCIENCES↗
Characterization of solid particle candidates for application in thermal energy storage and concentrating solar power systems
Thermal energy storage (TES) enables concentrating solar power to remain competitive in the renewable energy mix by firming up intermittent solar resource and providing grid services such as load shifting. Free from siting constraints, stand-alone TES systems show promise as a low-cost alternative to traditional pumped-storage hydropower or compressed air energy storage. At the core of all TES technologies is a storage medium, the selection of which governs many aspects of system design and operation. Although the majority of commercial installations utilize molten salts, solid particles can demonstrate stability over wider temperature ranges. This amounts to increased energy storage densities and corresponding reductions in system cost which is essential in achieving low-cost energy storage. In this work, eight solid particle candidates are systematically identified and screened for application in a specific particle-TES system. The five most promising candidates (CARBO CP and HSP, calcined flint clay (CFC), brown fused alumina (BFA), and silica sand) are further characterized by size and morphology for fluidization suitability, flowability for particle transport, and thermal stability. Calcined flint clay and brown fused alumina are eventually down-selected due to thermal instability at the target operational temperature of 1200 °C. Although the physical characteristics of CARBO outperform silica sand in all categories examined, the marginal performance gains are considered insufficient to justify the additional media cost so silica sand is selected as the leading candidate. Within the silica sand (α-quartz) space, the high end of Geldart Group B particles is identified to satisfy the target fluidization regime for the application of interest without compromising particle flowability. Here, in focused testing, Silica 460 is shown to exhibit sufficient stability through long-duration (500-hour) thermal and cyclic testing (1200 °C), 10-hour testing at 1400 °C, and in contact with candidate refractory containment materials. Finally, an average heat capacity of 1.1 J/g∙ °C is measured over 300-1200 °C with a quartz inversion enthalpy (ΔH α-β ) of 10.7J/g.
14 SOLAR ENERGY↗
Tuning cellulose pyrolysis chemistry: selective decarbonylation via catalyst-impregnated pyrolysis
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bio-inspired↗
Fluid-based gating mechanism with tunable multiphase selectivity and antifouling behavior
A gating mechanism that uses a capillary stabilized liquid as a reversible, reconfigurable gate that fills and seals pores in the closed state, and creates a non-fouling, liquid-lined pore in the open state is disclosed. Theoretical modeling and experiments demonstrate that for each transport substance, the gating threshold—the pressure needed to open the pores—can be rationally tuned over a wide pressure range. This enables realizing in one system differential response profiles for a variety of liquids and gases, even letting liquids flow through the pore while preventing gas from escaping. These capabilities allow dynamic modulation of gas-liquid sorting and to separate multi-phase mixtures, with the liquid lining ensuring sustained antifouling behavior. Because the liquid gating strategy enables efficient short-term and long-term operation and can be applied to a variety of pore structures and membrane materials, and to nano, micro as well as macroscale fluid systems, the gating systems is useful in a wide range of applications.
36 MATERIALS SCIENCE↗
Identification of Climatological Representative Days in the Mid-Atlantic for High-Fidelity Offshore Wind Energy Modeling
The goal of reaching 30 GW of offshore wind energy by 2030 becomes more realistic with the continued approval of offshore wind energy areas by the Biden Administration. In the Mid-Atlantic, where wind energy projects are in the most advanced stages of development, there is increased research focus on the eventual interaction of these wind farms. These interactions, in the form of wakes and cluster wakes, or wakes from multiple wind farms, could have detrimental effects on power production and forecastability for downwind wind farms (Pryor et al. 2022, Golbazi et al. 2022, Rosencrans et al. 2023). To help alleviate these issues, numerical simulations in the form of numerical weather prediction (NWP) and large eddy simulations (LES) can provide insight into when cluster wake situations may occur, but running such simulations can be expensive and difficult to run for multiple years. In this study, we leverage and build upon existing techniques in the literature (Fischereit et al. 2022) to identify climatologically representative days for wind energy areas in the Mid-Atlantic where conditions would promote cluster wake situations. We select meteorological variables (wind speed, wind direction, atmospheric stability, boundary-layer height, TKE) critical to understanding wind energy production and wake propagation. We then consider two different NWP datasets of varying spatial and temporal resolution: ERA5 provides data at hourly intervals from 1940 to present at 0.25 deg (31 km) spatial resolution (Hersbach et al. 2020), and the NOW-23 dataset provides data at 5-minute resolution for 21 years at 2-km spatial resolution (Bodini et al. 2020). Our first step is to compare these two datasets for an overlapping 21-year time period. Initial results show that the required number of days to represent the long-term climate increases with each additional variable considered. In their study of the German Bight, Fischereit et al. (2022) found that they could represent the long-term wind and wave climate in a "near-perfect" way with -180 days, by reaching a Perkins Skill Score (PSS) of 0.9; our investigation of the mid-Atlantic wind resource region with ERA5 and NOW-23 data suggests that we will need -100 days to reach a PSS of 0.9. As we expand our parameter space to include multiple variables, the number of required days will likely grow. These results will ultimately be used to select case studies to best represent cluster wake conditions that apply to this region for the lifetime of likely wind farms in this mid-Atlantic region.
clusterwakes↗