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At least 739 records · Page 41

Integrated Reference Electrodes in Anion-Exchange-Membrane Electrolyzers: Impact of Stainless-Steel Gas-Diffusion Layers and Internal Mechanical Pressure

Alkaline-membrane electrolyzers operating in pure water might provide scalable low-cost H 2 production but currently lag in performance and durability compared to commercial technologies. Typically, membrane–electrode assemblies (MEAs) are optimized in electrolyzers by changing one parameter at a time and assessing the resulting system performance via two-electrode polarization and impedance measurements. These approaches are limited in their ability to assign performance changes and durability to specific electrodes or processes. We integrate a reference electrode with the MEA to separate anode and cathode responses in both polarization and impedance measurements. Here we illustrate the power of the approach by showing how the fiber diameter of stainless-steel gas-diffusion layers (GDLs) affects performance solely at the anode, while changing the thickness of the cathode GDL simultaneously affects the performance of the anode and cathode due to changes in internal pressure from mechanical compression. This finding was obscured in conventional two-electrode measurements. The work thus guides both high-performance alkaline-membrane water-electrolyzer development and illustrates a useful strategy to study structure–activity relationships in the MEA.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Microstructure and diffusion behavior of uranium fuel with minor additives

Fission product lanthanides in metallic fuels are known to cause adverse fuel-cladding chemical interaction (FCCI). Tin (Sn) and palladium (Pd) are being explored as the potential additives to reduce or mitigate lanthanide-induced FCCI by forming stable Sn-Ln and Pd-Ln compounds. The current study is an investigation of the fuel alloys, U–4Sn, U–4Sn-4Ln, U–4Pd, and U–4Pd-4Ln (wt. %), and their diffusion behaviors with Fe. Microstructural analysis was performed using scanning electron microscopy (SEM). Further, the binary phases in the UPd and USn alloys are identified as UPd 3 and suspected U 2 Sn, where U 2 Sn is unknown in the literature. The binary phases in the UPdLn alloy are identified as PdLn and Pd-rich Pd-Ln (Pd 4 Ln 3 and Pd 3 Ln 2 ), and in the USnLn alloy is SnLn. Diffusion of Fe with these binary phases is insignificant compared to the diffusion with U. The Ln-induced FCCI can be mitigated by the additives.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fabrication of Lanthanum Telluride 14-1-11 Zintl High-Temperature Thermoelectric Couple

The development of more efficient thermoelectric couple technology capable of operating with high-grade heat sources up to 1,275 K is key to improving the performance of radioisotope thermoelectric generators. Lanthanum telluride La3-xTe4 and 14-1-11 Zintls (Yb14MnSb11) have been identified as very promising materials. The fabrication of advanced high-temperature thermoelectric couples requires the joining of several dissimilar materials, typically including a number of diffusion bonding and brazing steps, to achieve a device capable of operating at elevated temperatures across a large temperature differential (up to 900 K). A thermoelectric couple typically comprises a heat collector/ exchanger, metallic interconnects on both hot and cold sides, n-type and ptype conductivity thermoelectric elements, and cold-side hardware to connect to the cold-side heat rejection and provide electrical connections. Differences in the physical, mechanical, and chemical properties of the materials that make up the thermoelectric couple, especially differences in the coefficients of thermal expansion (CTE), result in undesirable interfacial stresses that can lead to mechanical failure of the device. The problem is further complicated by the fact that the thermoelectric materials under consideration have large CTE values, are brittle, and cracks can propagate through them with minimal resistance. The inherent challenge of bonding brittle, high-thermal-expansion thermoelectric materials to a hot shoe material that is thick enough to carry the requisite electrical current was overcome. A critical advantage over prior art is that this device was constructed using all diffusion bonds and a minimum number of assembly steps. The fabrication process and the materials used are described in the following steps: (1) Applying a thin refractory metal foil to both sides of lanthanum telluride. To fabricate the n-type leg of the advanced thermoelectric couple, the pre-synthesized lanthanum telluride coupon was diffusion bonded to the metal foil using a thin adhesion layer. (2) Repeating a similar process for the 14-1-11 Zintl p-type leg of the advanced thermoelectric couple. (3) Bonding thick CTE-matched metal plates on the metallized lanthanum telluride and Yb14MnSb11 to form the hot and cold sides of the thermoelectric couple. The calculated conversion efficiency of such an advanced couple would be about 10.5 percent, about 35 percent better than heritage radioisotope thermoelectric technology that relies on Si-Ge alloys. In addition, unlike Si-Ge alloys, these materials can be combined with many other thermoelectric materials optimized for operation at lower temperatures to achieve conversion efficiency in excess of 15 percent (a factor of 2 increase over heritage technology).

Ravi, Vilupanur A.↗

Diffusion and utilization of scientific and technological knowledge within state and local governments

The state-of-the-art is reviewed concerning current knowledge of processes by which technological innovation and scientific information are disseminated among state and local governments. The effectiveness of various mechanisms, strategies, and approaches by which federal agencies have sought to transfer technology to state, regional, and city governments are assessed. It is concluded that the existing relationships between the state and local governments, and the scientific communities are not adequate.

Feller, I.↗

Current legal and institutional issues in the commercialization of phosphoric acid fuel cells

Legal and institutional factors affecting the development and commercial diffusion of phosphoric acid fuel cells are assessed. Issues for future research and action are suggested. Perceived barriers and potential opportunities for fuel cells in central and dispersed utility operations and on-site applications are reviewed, as well as the general concept of commercialization as applied to emerging energy technologies.

Nimmons, J. T.↗

Volatility of Common Protective Oxides in High-Temperature Water Vapor: Current Understanding and Unanswered Questions

Many structural materials rely on the formation of chromia, silica or alumina as a protective layer when exposed in high temperature oxidizing environments. The presence of these oxide layers provides a protective diffusion barrier which slows down further oxidation. In atmospheres containing water vapor, however, reactions to form volatile hydroxide species occur which remove the surface oxide, thus, lowering the protective capability of the oxide scale. This paper summarizes the current understanding of volatility of chromia, silica and alumina in water vapor containing combustion environments. In addition unanswered questions in each system are discussed. Th current paper represents an update on the considerable information learned in the past five years for these systems.

Opila, Elizabeth J.↗

Effects of Fuel Preheat on Soot Formation in Microgravity Laminar Diffusion Flames

Nonbuoyant flames offer themselves as an attractive and promising platform to gain a better understanding of soot mechanisms. The effects of buoyancy can be eliminated temporarily in drop towers which sustain brief intervals of reduced gravity-typically lower than 10(exp -3)g- extending up to several seconds at a time. Microgravity facilities have been employed to show that nonbuoyant flames are longer, wider and sootier than their normal-gravity counterparts. Sunderland et al. recently verified the existence of smoke point in laminar nonbuoyant flames. As reported, microgravity flames operating above their smoke point displayed a blunt tip and much broader soot-containing regimes in comparison to their buoyant counterparts. Mortazavi et al. established that residence times in microgravity laminar jet diffusion flames with Re=0(100) tend to be proportional to burner diameter and inversely proportional to burner exit velocity. This offers the capability to alter residence times in nonbuoyant laminar jet diffusion flames when varying the burner exit diameters and velocities. Megaridis et al. presented a quantitative definition of the soot-field structure within laminar microgravity jet diffusion flames which operated well above their smoke point. The experimental methodology involved a full-field laser-light extinction technique and jet diffusion flames of nitrogen-diluted (50% vol.) acetylene fuel burning in quiescent air at atmospheric pressure. The work was conducted at the 2.2s drop tower of the NASA Lewis Research Center (NASA-LeRC). Parallel work on 1-g flames was also presented in (6) to facilitate comparisons on the effect of gravity on the soot fields. As reported, the soot spatial distributions in 0-g flames did not change in a detectable manner after 1s within a typical 2.2s experiment. During that period, the soot field was shown to sustain a pronounced annular structure throughout the luminous nonbuoyant-flame zone. The maximum soot volume fraction measured at 0-g was nearly a factor of two higher than that at 1-g, thus confirming the enhanced sooting tendency of nonbuoyant flames. Greenberg and Ku presented a similar study and reported trends that matched those of for the 50% (vol.) nitrogen-diluted acetylene fuel. Furthermore, they examined pure acetylene flames and reported similar trends with respect to the influence of gravity on maximum soot volume fractions and flame cross-section-averaged soot loadings. Both studies clearly demonstrated the improved spatial resolution of microgravity flames compared to their normal-gravity counterparts. The current study evaluates the influence of moderate fuel preheat on soot formation within 0-g laminar gas jet diffusion flames. While fuel temperature variations have little influence on residence times in 1-g, they have a much more significant effect in 0-g. The primary objective of this program is to quantify this effect and its consequences on sooting by comparing soot volume fraction distributions under preheated and unpreheated-fuel conditions. Furthermore, the current work aims at expanding the limited soot database available for nonbuoyant flames. Soot fields in such flames can be used to perform additional tests of recently developed soot sub-models which have the potential to become powerful predicting tools in combustion design.

Konsur, Bogdan↗

Zonal magnetic fields regulate nonlinear edge-localized-mode dynamics via self-consistent force balance

Edge-localized modes (ELMs) eject intense bursts of heat and particles that threaten plasma-facing components in fusion reactors. Nonlinear full-torus BOUT++ simulations show that turbulence-driven zonal magnetic fields (ZMFs) play an essential role in nonlinear ELM evolution by maintaining self-consistent force balance. Zonal flows mitigate the initial crash through shear but do not prevent continued radial transport. When ZMFs are self-consistently included, turbulence-driven zonal currents modify the parallel current distribution and magnetic tension and are associated with a reduction of the axisymmetric (𝑛 = 0) perturbed radial force imbalance. This coincides with a transition from convective, bursty propagation to more localized, diffusive transport. Similar behavior is observed across the regimes considered, including both resistive-ballooning and peeling-ballooning cases. Finally, associated signatures, including radial electric field shear and parallel current redistribution, provide experimentally accessible diagnostics for present devices and ITER-relevant conditions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Low- and medium-energy galactic gamma-ray observations

Observation of 0.2 to 100 MeV-diffuse gamma-radiation emitted from a galaxy provides information on the intensities of 5 to 50 MeV/nucleon cosmic-rays and approximately less than 50-MeV electrons in interstellar space. Recent measurements of gamma-rays emitted from the galactic center region provide evidence for a diffuse continuum between 10 and 100 MeV, which is dominant over the pi-decay emission generated in high-energy nuclear collisions. The intensities of the recently reported nuclear line gamma-rays, also observed in the direction of the galactic center, require the presence of intense fluxes of low energy cosmic rays in the inner galaxy if the gamma-ray are produced on a galactic scale. Current detection techniques for 0.1 to 100 MeV gamma-ray measurements are summarized, and their capabilities for measuring the diffuse galactic emission are evaluated.

Share, G. H.↗

Encapsulated diffusion of sulphur into InP

This talk outlines a simple process for the fabrication of n(+)-p solar cells in indium phosphide. Large area cells (greater than 0.25 sq cm) have been made by this process, with a photovoltaic conversion efficiency of 15.21 percent under AM0 conditions of illumination. An ideality factor of 1.1 and a saturation current density of 8 x 10 to the minus 15th power A/sq cm have been observed for these cells. The technique for cell fabrication involves the diffusion of sulfur into InP by an open tube process, and gives highly reproducible results from run to run. A vacuum-deposited layer of gallium sulphide (Ga2S3) was used as the source for sulfur diffusion, with a chemically vapor deposited SiO2 cap layer to prevent decomposition of the InP surface during heat treatment. Diffusions were carried out in a flowing nitrogen ambient at 585 to 708 C, and characterized by their surface carrier concentration and the diffusion constant. The diffusion profile for sulfur in InP is estimated to be of the complementary error function type. The activation energy of the diffusion was estimated to be 1.94 eV. The technique described here is ideally suited for the fabrication of shallow n(+)-p junctions in InP, and has been used for space-borne solar cells.

Parat, K. K.↗

Ion Transport and Crystal Rotation in Plastic Crystal Electrolytes Under Applied Electric Fields

Organic ionic plastic crystal electrolytes, containing a plastic crystal and lithium salt, offer a potential balance between mechanical and electrochemical properties for solid state lithium-ion battery electrolytes. These electrolytes contain multiple mobile ionic species (three or four), resulting in complex transport mechanisms which have not yet been established. Plastic crystals are defined by long-range positional order and short-range rotational disorder. It is therefore necessary to quantify changes in the local crystal structure of the electrolyte as current flows through it. Herein, we examine the electrochemical properties of pyrrolidinium-based plastic crystal electrolytes containing lithium salt and zwitterion additives, including measurements of current fraction and limiting current. We obtain species-specific insight into electrolyte transport using pulsed-field gradient nuclear magnetic resonance spectroscopy and find that, while the zwitterion additive increases ionic conductivity, it decreases lithium diffusivity with respect to other ionic components. With operando spatiotemporally resolved wide-angle X-ray scattering we observe location-specific crystal rotations due to the passage of ionic current. In conclusion, we posit that reducing energy dissipation due to rotation is essential for using plastic crystal electrolytes in practical applications.

Yap, Kyra M. K. [University of California, Berkele↗

LANL Meteorology Program Self-Assessment 2025 Update

The LANL Meteorological (Met) Program has been subject to several external reviews over the past 19 years. The DOE Meteorological Coordinating Council (DMCC) conducted an initial Met Program Site Assist Visit (SAV) in August 2006 (DMCC 2006). A follow-up SAV in August 2015 assessed progress (DMCC 2015), and in June 2023, the DOE Meteorological Subcommittee (DMSC), successor to the DMCC, conducted a second follow-up SAV (DMSC 2023), in which the Met Program was evaluated relative to the following 8 high-level questions: • What is the state of the meteorological services provided to its customers? • What is the quality of meteorological data provided to its customers and is it adequate and available to meet all customer needs? • What is the quality of atmospheric transport and diffusion modeling provided to its customers and is it applicable to complex wind flow patterns at LANL? • Are the current and future meteorological service customers being serviced appropriately? • Are there adequate human resources to meet present and future program customer needs and are they being appropriately leveraged? • Are existing instrumentation, facilities, and systems adequate to meet present and future customer needs? • Are LANL meteorological services conducted in an efficient, cost-effective manner? • Is meteorological data used to ensure safety & health of LANL personnel? More specific evaluations were performed relative to 23 performance objectives extracted from the ANSI/ANS-3.11- 2024 national standard and 14 separate performance objectives associated with consequence assessment and atmospheric transport and diffusion modeling in the consequence assessment element of DOE G 151.1-1B. In 2023, the DMSC SAV Team also reviewed the status of each of the 18 remaining recommendations from its 2015 SAV. Based on this review, DMSC stated in its Exit Briefing that the LANL meteorological program has gotten much stronger and more robust since 2015 and now represents one of the better managed programs within the DOE complex.

54 ENVIRONMENTAL SCIENCES↗

Diffuse Radiation Forcing Constraints on Gross Primary Productivity and Global Terrestrial Evapotranspiration

Abstract The diffuse radiation fertilization effect—the increase in plant productivity in the presence of higher diffuse radiation ( K ↓,d )—is an important yet understudied aspect of atmosphere‐biosphere interactions and can modify the terrestrial carbon, energy, and water budgets. The K ↓,d fertilization effect links the carbon cycle with clouds and aerosols, all of which are large sources of uncertainties for our current understanding of the Earth system and for future climate projections. Here we establish to what extent observational and modeling uncertainty in sunlight's diffuse fraction ( k d ) affects simulated gross primary productivity (GPP) and terrestrial evapotranspiration ( λE ). We find only 48 eddy covariance sites with simultaneous sufficient measurements of K ↓,d with none in the tropical climate zone, making it difficult to constrain this mechanism globally using observations. Using a land modeling framework based on the latest version of the Community Land Model, we find that global GPP ranges from 114 Pg C year −1 when using k d forcing from the Modern‐Era Retrospective analysis for Research and Applications, version 2 reanalysis to a ∼7% higher value of 122 Pg C year −1 when using the Clouds and the Earth's Radiant Energy System satellite product, with especially strong differences apparent over the tropical region (mean increase ∼9%). The differences in λE , although smaller (−0.4%) due to competing changes in shaded and sunlit leaf transpiration, can be greater than regional impacts of individual forcing agents like aerosols. Our results demonstrate the importance of comprehensively and systematically validating the simulated k d by atmosphere modules as well as the response to differences in k d within land modules across Earth System Models.

54 ENVIRONMENTAL SCIENCES↗

Coordinated Studies of Magnetospheric/Ionospheric Coupling and Dynamics in the Diffuse Aurora

The results of the studies carried out under the grant are described in detail in the following publications: Atmospheric Response in Aurora experiment: Observations of E and F region neutral winds in a region of postmidnight diffuse aurora; Walterscheid, Modified geostrophy in the thermosphere, ARIA II neutral flywheel-driven field-aligned currents in the postmidnight sector of the auroral oval: A case study; Observations of unstable atmospheric shear layers in the lower E region in the post-midnight auroral oval; and Depletion of oxygen in aurora: Evidence for a local mechanism. The objective of the Atmospheric Response in Aurora (ARIA) experiment was to measure the response of the E-region neutral flow to substorm activity in the post-midnight sector of the auroral oval. To this end, neutral wind profiles were obtained from a series of four sets of rocket flights using the chemical release technique. The measurements covered conditions ranging from quiet to disturbed. A consistent feature of the observed winds in disturbed conditions is the presence of an E-region jet located between approximately 110 and 120 km altitude. The profiles presented here show that the neutral wind speeds near 110-120 km altitude increase and the hodographs become more elongated or linear in response to higher magnetic activity levels. The wind speeds decrease and the hodographs become more circular as the activity level decreases. The presence of a wind maximum implies shears both above and below. The observations consistently show larger shears below the peak and smaller shears above. In fact, the bottom-side shears during disturbed conditions have Richardson numbers close to or below the critical value of 0.25 suggesting that the flow is highly unstable in that height range. The instability is expected to produce waves, turbulence, and enhanced diffusivity.

Larsen, M. F.↗

Electron-Beam-Related Studies of Halide Perovskites: Challenges and Opportunities

Electron beam microscopy and related characterization techniques play an important role in revealing the microstructural, morphological, physical, and chemical information of halide perovskites and their impact on associated optoelectronic devices. However, electron beam irradiation usually causes damage to these beam-sensitive materials, negatively impacting their device performance, and complicating this interpretation. Here, the electron microscopy and spectroscopy techniques are reviewed that are crucial for the understanding of the crystallization and microstructure of halide perovskites. In addition, special attention is paid to assessing and mitigating the electron beam-induced damage caused by these techniques. Since the halide perovskites are fragile, a protocol involving delicate control of both electron beam dose and dose rate, coupled with careful data analysis, is key to enable the acquisition of reliable structural and compositional information such as atomic-resolution images, chemical elemental mapping and electron diffraction patterns. Limiting the electron beam dose is critical parameter enabling the characterization of various halide perovskites. Novel methods to unveil the mechanisms of device operation, including charge carrier generation, diffusion, and extraction are presented in scanning electron microscopy studies combined with electron-beam-induced current and cathodoluminescence mapping. Future opportunities for electron-beam-related characterizations of halide perovskites are also discussed.

36 MATERIALS SCIENCE↗

Facet‐Selective Deposition of Ultrathin Al 2 O 3 on Copper Nanocrystals for Highly Stable CO 2 Electroreduction to Ethylene

Abstract Catalysts based on Cu nanocrystals (NCs) for electrochemical CO 2 ‐to‐C 2+ conversion with high activity have been a subject of considerable interest, but poor stability and low selectivity for a single C 2+ product remain obstacles for realizing sustainable carbon‐neutral cycles. Here, we used the facet‐selective atomic layer deposition (FS‐ALD) technique to selectively cover the (111) surface of Cu NCs with ultrathin Al 2 O 3 to increase the exposed facet ratio of (100)/(111), resulting in a faradaic efficiency ratio of C 2 H 4 /CH 4 for overcoated Cu NCs 22 times higher than that for pure Cu NCs. Peak performance of the overcoated catalyst (Cu NCs/Al 2 O 3 ‐10C) reaches a C 2 H 4 faradaic efficiency of 60.4 % at a current density of 300 mA cm −2 in 5 M KOH electrolyte, when using a gas diffusion electrode flow cell. Moreover, the Al 2 O 3 overcoating effectively suppresses the dynamic mobility and the aggregation of Cu NCs, which explains the negligible activity loss and selectivity degradations of Cu NCs/Al 2 O 3 ‐10C shown in stability tests.

Li, Hui↗

Facet-Selective Deposition of Ultrathin Al 2 O 3 on Copper Nanocrystals for Highly Stable CO 2 Electroreduction to Ethylene.

Catalysts based on Cu nanocrystals (NCs) for electrochemical CO 2 -to- 2+ conversion with high activity have been a subject of considerable interest, but poor stability and low selectivity for a single C 2+ product remain obstacles for realizing sustainable carbon-neutral cycles. In this study, we used the facet-selective atomic layer deposition (FS-ALD) technique to selectively cover the (111) surface of Cu NCs with ultrathin Al 2 O 3 to increase the exposed facet ratio of (100)/(111), resulting in a faradaic efficiency ratio of C 2 H 4 /CH 4 for overcoated Cu NCs 22 times higher than that for pure Cu NCs. Peak performance of the overcoated catalyst (Cu NCs/Al 2 O 3 -10C) reaches a C 2 H 4 faradaic efficiency of 60.4 % at a current density of 300 mA cm -2 in 5 M KOH electrolyte, when using a gas diffusion electrode flow cell. Moreover, the Al 2 O 3 overcoating effectively suppresses the dynamic mobility and the aggregation of Cu NCs, which explains the negligible activity loss and selectivity degradations of Cu NCs/Al 2 O 3 -10C shown in stability tests.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A dynamic variational multiscale method on unstructured meshes for stationary transport problems

Here, this paper presents a variational multiscale (VMS) based finite element method where the stabilization parameter is computed dynamically. The current dynamic procedure takes in a general structure/form of the stabilization parameter with unknown coefficients and computes them dynamically in a local fashion resulting in a dynamic VMS-based finite element method. Thus, a static stabilization parameter with pre-defined coefficients is not needed. A variational Germano identity (VGI) based local procedure suitable for unstructured meshes is developed to perform the dynamic computation in a local fashion. The local VGI based procedure is applied for each interior vertex in the mesh and unknown coefficients are first determined locally at each vertex, and subsequently, for each element a maximum value is taken over the vertices of the element. To make the current procedure practical, a coarser secondary solution is constructed from the primary coarse-scale solution, which is done locally over a patch of elements around each interior vertex. Further, averaging steps are employed to make the local dynamic procedure robust. Currently, the new dynamic VMS formulation is applied to steady problems governed by the advection-diffusion and incompressible Navier-Stokes equations in both 1D and 2D to demonstrate its efficacy and effectiveness.

97 MATHEMATICS AND COMPUTING↗