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At least 649 records · Page 36

Evaluation of Neutron-Radiation Tolerance of Lithium Indium Diselenide Semiconductors

Herein we discuss lithium indium diselenide (LISe) as a semiconductor that holds promise for neutron imaging sensor technologies because of its high neutron absorption efficiency and its corresponding ability to discriminate between gamma rays and neutrons. However, being a semiconductor, LISe may not be sufficiently radiation hard for practical application in radiation hard environments. Therefore, a systematic evaluation of the changes in material and electronic properties of LISe after high neutron fluence exposures is investigated. Herein, the characterization methods are utilized which included UV–vis, X-ray diffraction, radioluminescence, Raman, fourier transform infrared spectroscopy (FTIR), current–voltage, and neutron sensing. Characteristics of LISe material that appeared in the literature are identified herein along with several that are expected to appear based on theoretical analyses. The results obtained show clear changes in the material properties of LISe after neutron exposure up to a fluence of 10 16 n cm -2 . However, LISe is still able to sense neutrons above the background at 10 16 n cm -2 , suggesting that LISe may be suitable for use in neutron imaging sensors at neutron imaging facilities.

36 MATERIALS SCIENCE↗

Conical-reflector antennas.

The mechanical advantages of a singly curved conical reflector are demonstrated by the experimental test of a furlable 1.83 m conical-Gregorian antenna at 16.33 GHz. The measured gain of 47.5 dB corresponds to a net efficiency of over 57%. A ray-optics analysis of conical-reflector antennas is presented, and data useful in the design of conical antennas are given. The conical-Gregorian antenna, in which a subreflector is used in conjunction with a conventional horn feed, is considered in detail. A physical-optics analysis of the conical-Gregorian antenna is used to investigate diffraction and other effects, and to analytically confirm the high performance of the antenna.

Ludwig, A. C.↗

Printed graphene oxide-based membranes for gas separation and carbon capture

Graphene oxide (GO)-based separation membranes have demonstrated the great potential to separate molecules and ions by the interlayer spacing with tunable nano-sized channels. The scalable fabrication of GO-based gas separation membranes, however, remains challenging, although a few preparation approaches have been reported. Here in this work, we present for the first time that the co-solvent ink-jet printing, as a fast and scalable method, can be utilized for scalable GO-based gas separation membrane preparation. Large-area (>100 cm 2 ), ultrathin, and high-quality GO membrane was successfully deposited on commercial polysulfone (PS) support, and characterized by scanning electron microscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, and X-ray diffraction, et al., Selective hydrogen (H 2 ) and helium (He) transport over carbon dioxide (CO 2 ) and nitrogen (N 2 ) was demonstrated for the printed GO membrane. To further explore the separation potential of the printed GO-based gas membrane, additives for facilitated molecular transport were incorporated during the membrane printing process. By inserting CO 2 -philic agents into the printed GO membrane, highly efficient separation of CO 2 from N 2 was achieved with CO 2 /N 2 selectivity of 70 and CO 2 permeance as high as 2,500 GPU. The strategy proposed here may provide guidance for large-scale GO-based gas separation membrane production and a versatile approach for applying other functional 2-dimensional materials towards the membrane separation application.

42 ENGINEERING↗

Revisiting the initial irreversible capacity loss of LiNi 0.6 Co 0.2 Mn 0.2 O 2 cathode material batteries

Layered LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) attracts widespread attention primarily due to its potential for high energy density and moderate thermal stability. However, the low initial coulombic efficiency (ICE) of the material limits the maximum utilization of their capacity. The capacity loss in the first cycle occurs under 4.0V and keep almost constant are considered as common characteristics for NCM-based materials. A clear cognition on the initial capacity loss may light the way to improve the practical reversible capacity of NCM622 at 4.0V. Conducting operando X-ray diffraction during galvanostatic charge/discharge cycling at different temperature (25 degrees C, 45 degrees C and 60 degrees C) and different current (0.1C, 0.01C, 1C=120 mA g -1 ) in the voltage range of 2.7-4.0V, we find that only 8% of the measured initial irreversible capacity loss is associated with parasitic reactions that form cathode/electrolyte interface, and that the dominant contributors include the slow Li + diffusion kinetics (similar to 46% contribution) and irreversible O3/H1-3 phase transition (similar to 46% contribution). Finally, this semi-quantitative study provides new insight on initial capacity loss, guiding further targeted modification and fully utilization of NCM622.

25 ENERGY STORAGE↗

The importance of ester cleavage in the butylamine pretreatment of hybrid poplar

Butylamine is an effective in-and-out pretreatment solvent for hybrid poplar. It penetrates the cell walls and breaks ester cross-linkages, facilitating lignin release and improving enzymatic digestion. This work explores the “in-and-out” pretreatment of hybrid poplar with butylamine as a distillable protic solvent and reagent. The butylamine solvent can be removed by vacuum distillation with >95% solvent removal in all cases, providing a valuable scheme for efficient solvent recovery and recycling. Running the reaction with neat butylamine at 140 °C for 3 hours results in high yields of monosaccharides (90% glucose and 71% xylose) after enzymatic digestion, and a good tolerance to water content with no significant reduction in glucose yield up to an 8 : 1 water : butylamine ratio. We investigate the mechanisms of this pretreatment using powder X-ray diffraction, thermogravimetric analysis, fluorescence microscopy, elemental analysis, solid state and solution state nuclear magnetic spectroscopy to observe chemical and material markers of the pretreatment chemistry. The results suggest that the butylamine leaves the macro and microstructural properties of the lignocellulose relatively unaltered, but conducts targeted ester cleavage chemistry to remove cross-links between the various biopolymers and partially solubilize the lignin component of the biomass. These findings should act to guide future development of pretreatment chemistry for the development of biorefinery processes, and assist in the utilization of biomass as a starting point for chemical syntheses.

Palasz, Joseph M↗

Prototype laser-diode-pumped solid state laser transmitters

Monolithic, diode-pumped Nd:YAG ring lasers can provide diffraction-limited, single-frequency, narrow-linewidth, tunable output which is adequate for use as a local oscillator in a coherent communication system. A laser was built which had a linewidth of about 2 kHz, a power of 5 milliwatts, and which was tunable over a range of 30 MHz in a few microseconds. This laser was phase-locked to a second, similar laser. This demonstrates that the powerful technique of heterodyne detection is possible with a diode-pumped laser used as the local oscillator. Laser diode pumping of monolithic Nd:YAG rings can lead to output powers of hundreds of milliwatts from a single laser. A laser was built with a single-mode output of 310 mW. Several lasers can be chained together to sum their power, while maintaining diffraction-limited, single frequency operation. This technique was demonstrated with two lasers, with a total output of 340 mW, and is expected to be practical for up to about ten lasers. Thus with lasers of 310 mW, output of up to 3 W is possible. The chaining technique, if properly engineered, results in redundancy. The technique of resonant external modulation and doubling is designed to efficiently convert the continuous wave, infrared output of our lasers into low duty-cycle pulsed green output. This technique was verified through both computer modeling and experimentation. Further work would be necessary to develop a deliverable system using this technique.

Kane, Thomas J.↗

Effects of Hydrogen Redistribution at High Temperatures in Yttrium Hydride Moderator Material

We report advanced materials development, manufacturing, and modeling capabilities for innovative reactor designs support nuclear security and mission-focused science through enhanced technology for safer and more efficient and secure production of nuclear energy. The high temperature moderator material yttrium hydride poses a significant enhancement in small reactor design by thermalizing (slowing down) neutrons and decreasing the required fuel mass for a system. The research presented here supports understanding hydrogen distribution in yttrium hydride through: (1) the development of neutron-based hydrogen imaging and crystallographic characterization that allows us to understand fundamental diffraction behaviors and to observe changes in hydrogen distribution as a function of temperature and (2) subsequent neutron multiplication (reactivity) effects of changes in hydrogen distribution using measurement-based cross sections in a sample microreactor design. The main conclusions from the work are that: (1) hydrogen does not redistribute significantly below temperatures of 800°C in yttrium hydride and (2) hydrogen redistribution affects the reactivity slightly but not significantly.

36 MATERIALS SCIENCE↗

Quasi-optical beam tracing module development for millimeter-wave high-wavenumber collective scattering on the NSTX-U and EAST tokamaks

A Python3-based beam tracing code utilizing Quasi-Optics has been developed to track both incident and receiving beams in high-k collective millimeter wave scattering systems within magnetic fusion plasmas. In contrast to existing ray tracing codes that solely consider refraction, this beam tracing code incorporates diffraction phenomena, providing a more comprehensive calculation. Here, this enhanced capability allows for a more accurate calculation of the scattering volume and spatial resolution in high-k collective scattering systems, crucial for evaluating system performance and facilitating data analysis. Unlike Geometrical Optics, Quasi-Optics employs the complex eikonal method, representing a Gaussian beam as a collection of coupled rays to accurately preserve diffraction characteristics. The developed code is intended for application in NSTX-Upgrade and EAST high-k beam tracing analyses, targeting frequencies of 693 GHz and 270 GHz, respectively. The high-k system's primary objective is the observation of electron-scale instabilities. Employing a symplectic integrator, the code ensures numerical accuracy, assessed through the conservation of the Hamiltonian. With its precision and efficiency, the code facilitates rapid inter-shot analyses.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Effect of Natural Fermentation of Sorghum on Resistant Starch Molecular Structure and Fermentation Property

Relevant research results have suggested that fermentation can increase the content of sorghum amylose chains and their retrogradation value. Therefore, this study explored the effect of fermentation pretreatment on the yield, digestibility, molecular structure, and in vitro fermentation property of sorghum-resistant starch by conducting fermentation pretreatment of sorghum and extracting the resistant starch from fermented sorghum with pressure-heat compound enzyme method. The results were as follows. After fermentation pretreatment, the yield of sorghum-resistant starch increased, the digestibility of sorghum-resistant starch reduced, the laminated structure size on the surface of the particles became more uniform, and the stacking mode became more neat and denser. The sorghum-resistant starch prepared before and after fermentation did not produce new chemical groups, and its functional group peak remained unchanged. After fermentation, the weight-average molecular weight of sorghum-resistant starch was elevated, and the percentage content of high- and low-molecular substances increased and decreased, respectively, compared with that of the unfermented sorghum-resistant starch. The percentage content of short-chain branches in the branched chain increased, whereas that of the long-chain branches decreased; the crystallinity of sorghum-resistant starch after fermentation decreased, and the intensity of X-diffraction peak changed slightly before and after fermentation. According to the results of the in vitro fermentation experiments, the fermentation broth of sorghum-resistant starch had the highest content of butyric acid and short-chain fatty acid. Research results reveal that, after fermentation pretreatment, sorghum-resistant starch presented increased yield, more complex molecular structure, heavier molecular weight and more uniform surface morphology, more efficient butyric acid generation, and greater fermentation rate than unfermented sorghum-resistant starch.

Ge, YunFei↗

Change of blaze wavelength as a function of position on the surface of a concave grating

Conventional ruling of a concave diffraction grating with blaze angle constant relative to the optical axis produces a grating whose blaze wavelength changes continuously with displacement across the face of the ruled area. A simple explanation of the effect is given in terms of geometrical optics, and quantitative expressions are developed that relate the expected blaze-wavelength shift to the grating constant and aperture ratio. Results are compared with experimental efficiency measurements, and the magnitude of the effect in a typical grating is discussed.

Michels, D. J.↗

Carbide-Modified Pd on ZrO2 as Active Phase for CO2-Reforming of Methane—A Model Phase Boundary Approach

Starting from subsurface Zr0-doped “inverse” Pd and bulk-intermetallic Pd0Zr0 model catalyst precursors, we investigated the dry reforming reaction of methane (DRM) using synchrotron-based near ambient pressure in-situ X-ray photoelectron spectroscopy (NAP-XPS), in-situ X-ray diffraction and catalytic testing in an ultrahigh-vacuum-compatible recirculating batch reactor cell. Both intermetallic precursors develop a Pd0–ZrO2 phase boundary under realistic DRM conditions, whereby the oxidative segregation of ZrO2 from bulk intermetallic PdxZry leads to a highly active composite layer of carbide-modified Pd0 metal nanoparticles in contact with tetragonal ZrO2. This active state exhibits reaction rates exceeding those of a conventional supported Pd–ZrO2 reference catalyst and its high activity is unambiguously linked to the fast conversion of the highly reactive carbidic/dissolved C-species inside Pd0 toward CO at the Pd/ZrO2 phase boundary, which serves the role of providing efficient CO2 activation sites. In contrast, the near-surface intermetallic precursor decomposes toward ZrO2 islands at the surface of a quasi-infinite Pd0 metal bulk. Strongly delayed Pd carbide accumulation and thus carbon resegregation under reaction conditions leads to a much less active interfacial ZrO2–Pd0 state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Impact of processing conditions on the film formation of lead-free halide double perovskite Cs 2 AgBiBr 6

Lead-free halide double perovskites with enhanced stability have gained attention as a promising environmentally friendly alternative to lead-based halide perovskites. Amongst different halide double perovskites, Cs 2 AgBiBr 6 has shown attractive optoelectronic properties and stability, making it a promising candidate for stable high-efficiency optoelectronic devices. Motivated by a data mining effort, we present here in this study the effects of different processing strategies on the microstructure and thin-film formation dynamics of Cs 2 AgBiBr 6 . We apply some of the most successfully used solvent engineering approaches from the halide perovskite research to halide double perovskites, namely antisolvent- and additive-assisted synthesis. Using in situ spectroscopy and diffraction, the film formation of Cs 2 AgBiBr 6 is investigated during spin coating, and the subsequent post-deposition thermal annealing. Dropping antisolvents during spin coating induces immediate supersaturation and crystallization of the wet film, whereas the time of dropping the antisolvent has implications on the film formation dynamics and the final microstructure. For additive (HBr)-assisted synthesis, we show how the addition of HBr affects colloid formation in solution and thus influences the crystallization pathway during thin-film processing. Finally, HBr additive simplifies synthesis in that it doesn't require solution and substrate preheating to obtain pinhole-free films even with higher thickness.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The first experimental evidence for improved nanomechanical properties of calcium silicate hydrate by polycarboxylate ether and graphene oxide

Graphene oxide (GO) efficiently enhances macroscale mechanical properties of cement-based materials. Yet the nanoscale reinforcing mechanism of GO for calcium silicate hydrate (C-S-H), the key binding phase of concrete, remains poorly understood. Moreover, how polycarboxylate ether (PCE)-based superplasticizers affect the nanomechanical properties of C-S-H remains unclear. The intrinsic mechanical properties of the nanocomposites are measured using high-pressure X-ray diffraction. The influences of GO and PCE on the local Ca and Si environments are probed using X-ray absorption spectroscopy. For the first time, we evidence that PCE-induced well-dispersed GO nanoplatelets strengthen the C-S-H basal planes, whereas poorly water-dispersed GO weakly interacts with basal planes and does not strengthen in plane Casingle bondO bonds. Both PCE and GO only slightly strengthen C-S-H's c-axis. Here, the bulk modulus of C-S-H/PCE/GO nanocomposite is 190% than pure C-S-H. Functional groups of PCE and GO prefer interacting with the Casingle bondO sheets of C-S-Hs instead of silicate tetrahedra.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Inhibit the strain accumulation for 5V spinel cathode by mitigating the phase separation during high voltage stage

LiNi 0.5 Mn 1.5 O 4 (LNMO) spinel cathode is a potential cathode material for high-power, low-cost lithium-ion batteries (LIBs) due to its low raw material cost, high operating voltage and efficient lithium-ion transport channel. However, LNMO suffers from structural stability due to the two-phase-transformation during charge/discharge process, leading to poor cycling performance. Here, to address the issues, we have constructed a homogeneous aggregated LNMO cathode with a multifaceted primary particle, namely the LNMO with single-crystal secondary particles (SSP LNMO). Ex situ and in situ characterizations including the synchrotron X-ray diffraction, the neutron diffraction and full pouch cell validated that the SSP LNMO exhibit a single solid-solution reactions with a restrained lattice evolution during the delithiation/lithiation process. This is in contrast to the normal LNMO cathode, which demonstrates a significant two-phase transition from spinel Li 1-x Ni 0.5 Mn 1.5 O 4 to rock-salt MnO 2 at high voltage. Therefore, the SSP LNMO has greatly improved cycle life compared to the normal LNMO cathode. Overall, this study demonstrates the possibility of constructing LNMO based on primary-grain morphology modulation to improve the intrinsic stability of LIBs.

25 ENERGY STORAGE↗

Heterointercalation in Chevrel-Phase Sulfides: A Model Periodic Solid for the Investigation of Chain Electron Transfer

Modulation of electron density localization on periodic crystal solids through electron transfer from interstitial cations can directly influence the bonding configurations of small-molecule intermediates at the catalyst binding site. This study presents the microwave-assisted solid-state synthesis of four heterointercalant Chevrel-phase (CP) sulfides with varying metal cation intercalants with compositional and electronic structure investigations of the electron density redistribution as a result of intercalation. The heterointercalant CP sulfides, with the general formula Cu x M y Mo 6 S 8 (where M = Cr, Mn, Fe, Ni; x, y = 1.5−2.5), are presented here for the probe reaction of electrochemical CO 2 reduction. A change in product selectivity is observed toward the production of methanol at low overpotentials of −0.5 V vs reversible hydrogen electrode (RHE), as a result of the intercalant combination present within the CP interstitial cavity. Structural confirmation of all materials was examined through Rietveld refinement of the powder X-ray diffraction (PXRD) data, high-resolution transmission electron microscopy (HR-TEM), and selected-area electron diffraction (SAED). Electron transfer from the intercalated metal cations to the Mo 6 S 8 cluster was investigated via X-ray photoelectron spectroscopy (XPS) of the intercalated metal cations and the chalcogenide cluster. Electron transfer was further confirmed through X-ray absorption analysis (XAS) of the K-edges of Mo and intercalants. Intermediate studies of electrochemical reduction of formaldehyde to methanol resulted in a faradaic efficiency of ∼78% methanol production on Cu x Ni y Mo 6 S 8 . The results presented herein identify distinct principles for materials design that can be utilized in other compositional spaces within the broad families of periodic crystal solids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

In-situ and wavelength-dependent photocatalytic strain evolution of a single Au nanoparticle on a TiO 2 film

Photocatalysis is a promising technique due to its capacity to efficiently harvest solar energy and its potential to address the global energy crisis. However, the structure–activity relationships of photocatalyst during wavelength-dependent photocatalytic reactions remains largely unexplored because it is difficult to measure under operating conditions. Here we show the photocatalytic strain evolution of a single Au nanoparticle (AuNP) supported on a TiO 2 film by combining three-dimensional (3D) Bragg coherent X-ray diffraction imaging with an external light source. The wavelength-dependent generation of reactive oxygen species (ROS) has significant effects on the structural deformation of the AuNP, leading to its strain evolution. Density functional theory (DFT) calculations are employed to rationalize the induced strain caused by the adsorption of ROS on the AuNP surface. These observations provide insights of how the photocatalytic activity impacts on the structural deformation of AuNP, contributing to the general understanding of the atomic-level catalytic adsorption process.

14 SOLAR ENERGY↗

Collaborative R&D with REEL Solar Inc (REEL) to Understand and Overcome Performance Limitations in CdTe Solar Cells: Cooperative Research and Development (Final Report)

This CRADA will focus on processing, advanced characterization, and testing of photovoltaic materials and devices to understand and improve REEL CdTe solar technology. This will include examining process variations and different buffer, absorber, and contact layers from REEL and NLR to maximize performance. The unique and diverse advanced characterization tools at NLR, such as time-resolved photoluminescence, capacitance-voltage measurements, electron beam scattered diffraction, cathodoluminescence, electron microscopy, TOF-SIMS, and other measurements will be applied to characterize REEL processing to improve understanding and guide experimental directions. Accelerated stability and potential induced degradation tests will be used to analyze metastability, short-and-long term degradation, and improve bankability. A second and major thrust this period will be joint development of Si/CdTe tandem solar cells to overcome industry wide terrestrial solar efficiency limits with the two lowest cost and manufacturable solar materials today. This will include developing novel transparent back contacts that can be incorporated into tandem structures and other novel solar applications, detailed analysis of designs and configurations for CdTe/Si tandem modules, and prototyping REEL CdTe Technology with Si bottom cells in tandem structures.

14 SOLAR ENERGY↗

Coherent Doppler Laser Radar: Technology Development and Applications

NASA's Marshall Space Flight Center has been investigating, developing, and applying coherent Doppler laser radar technology for over 30 years. These efforts have included the first wind measurement in 1967, the first airborne flights in 1972, the first airborne wind field mapping in 1981, and the first measurement of hurricane eyewall winds in 1998. A parallel effort at MSFC since 1982 has been the study, modeling and technology development for a space-based global wind measurement system. These endeavors to date have resulted in compact, robust, eyesafe lidars at 2 micron wavelength based on solid-state laser technology; in a factor of 6 volume reduction in near diffraction limited, space-qualifiable telescopes; in sophisticated airborne scanners with full platform motion subtraction; in local oscillator lasers capable of rapid tuning of 25 GHz for removal of relative laser radar to target velocities over a 25 km/s range; in performance prediction theory and simulations that have been validated experimentally; and in extensive field campaign experience. We have also begun efforts to dramatically improve the fundamental photon efficiency of the laser radar, to demonstrate advanced lower mass laser radar telescopes and scanners; to develop laser and laser radar system alignment maintenance technologies; and to greatly improve the electrical efficiency, cooling technique, and robustness of the pulsed laser. This coherent Doppler laser radar technology is suitable for high resolution, high accuracy wind mapping; for aerosol and cloud measurement; for Differential Absorption Lidar (DIAL) measurements of atmospheric and trace gases; for hard target range and velocity measurement; and for hard target vibration spectra measurement. It is also suitable for a number of aircraft operations applications such as clear air turbulence (CAT) detection; dangerous wind shear (microburst) detection; airspeed, angle of attack, and sideslip measurement; and fuel savings through headwind minimization. In addition to the airborne and space platforms, a coherent Doppler laser radar system in an unmanned aerial vehicle (UAV) could provide battlefield weather and target identification.

Kavaya, Michael J.↗