Stagnation-point convective heat transfer in frozen boundary layers.
Stagnation point convective heat transfer in frozen boundary layers to surfaces having widely differing catalytic activity in ionized flows
Pope, R. B.↗
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Stagnation-point convective heat transfer in frozen boundary layers.
Stagnation point convective heat transfer in frozen boundary layers to surfaces having widely differing catalytic activity in ionized flows
Pope, R. B.↗
Fabrication of tunnel junctions on niobium films.
Tunnel junctions with low background currents made by reacting active gas layer adsorbed on Nb film surface with Pb upper film to form barrier
Mullen, L. O.↗
Closing the Seasonal Ocean Surface Temperature Balance in the Eastern Tropical Oceans from Remote Sensing and Model Reanalyses
Residual forcing necessary to close the MLTB on seasonal time scales are largest in regions of strongest surface heat flux forcing. Identifying the dominant source of error - surface heat flux error, mixed layer depth estimation, ocean dynamical forcing - remains a challenge in the eastern tropical oceans where ocean processes are very active. Improved sub-surface observations are necessary to better constrain errors. 1. Mixed layer depth evolution is critical to the seasonal evolution of mixed layer temperatures. It determines the inertia of the mixed layer, and scales the sensitivity of the MLTB to errors in surface heat flux and ocean dynamical forcing. This role produces timing impacts for errors in SST prediction. 2. Errors in the MLTB are larger than the historical 10Wm-2 target accuracy. In some regions, a larger accuracy can be tolerated if the goal is to resolve the seasonal SST cycle.
Roberts, J. Brent↗
Low Temperature Activation of Methane on Metal-Oxides and Complex Interfaces: Insights from Surface Science
The abundance of inexpensive, natural gas has transformed the energy landscape, whereby revealing new possibilities for sustainable chemical technologies or impacting those that have relied on traditional fossil fuels. The primary component, methane, is underutilized and wastefully exhausted, leading to anthropogenic global warming. Historically, the manipulation of methane remained “ clavis aurea ,” an insurmountable yet rewarding challenge and thus the focus of intense research. This is primarily due to an inability to dissociate C–H bonds in methane selectively, which requires a high energy penalty and is an essential prerequisite for the direct conversion of methane into a large set of value-added products. The discovery of such processes would promise an energy gainful use of natural gas benefiting several essential chemical processes associated with C1 chemistry. This first C–H bond dissociation step of the methane molecule appears in numerous catalytic mechanisms as the rate-determining step or most essential barrier sequence for all subsequent steps that follow in the production of C–C, C–O, or C x –H y –O z bonds found in value added products. A main goal is to catalytically reduce the energy barrier for the first C–H bond dissociation to be able to achieve the activation of methane at low or moderate temperatures. As such there is great value in understanding the fundamental nature of the active sites responsible for bond breaking or formation and thus be able to facilitate better control of this chemistry, leading to the development of new technologies for fuel production and chemical conversion. Surface science studies offer enhanced perspectives for a careful manipulation of bonds over the last layer atoms of catalyst surfaces, an essential factor for the design of atomically precise catalysts and unravelling of the reaction mechanism. With the advent of new surface imaging, spectroscopy, and in situ tools, it has been possible to decipher the surface chemistry of complex materials systems and further our understanding of atomic active sites on the surfaces of metals, oxides, and carbides or metal–oxide and metal–carbide interfaces. The once considered near impossible step of C–H bond activation is now observed at low temperatures with high propensity over a collection of oxide, metal–oxide, and metal–carbide systems in a conventional or inverse configuration (oxide or carbide on metal). The enabling of C–H activation at low temperature has opened interesting possibilities for the specific production of chemicals such as methanol directly from methane, a step toward facile synthesis of liquid fuels. We highlight the most recent of these results and present the key aspects of active site configurations engineered from surface science studies which enable such a simple reactive event through careful manipulation of the last surface layer of atoms found in the catalyst structure. New concepts which help in the activation and conversion of methane are discussed.
36 MATERIALS SCIENCE↗
The Estimation Surface Latent Heat Flux Over the Ocean and its Relationship to Marine Atmospheric Boundary Layer (MABL) Structure
A new technique combining active and passive remote sensing instruments for the estimation of surface latent heat flux over the ocean is presented. This synergistic method utilizes aerosol lidar backscatter data, multi-channel infrared radiometer data and microwave scatterometer data acquired onboard the NASA P-3B research aircraft during an extended field campaign over the Atlantic ocean in support of the Lidar In-space Technology Experiment (LITE) in September of 1994. The 10 meter wind speed derived from the scatterometers and the lidar-radiometer inferred near-surface moisture are used to obtain an estimate of the surface flux of moisture via bulk aerodynamic formulae. The results are compared with the Special Sensor Microwave Imager (SSM/I) daily average latent heat flux and show reasonable agreement. However, the SSM/I values are biased high by about 30 W/sq m. In addition, the MABL height, entrainment zone thickness and integrated lidar backscatter intensity are computed from the lidar data and compared with the magnitude of the surface fluxes. The results show that the surface latent heat flux is most strongly correlated with entrainment zone top, bottom and the integrated MABL lidar backscatter, with corresponding correlation coefficients of 0.62, 0.67 and 0.61, respectively.
Palm, Stephen P.↗
The Estimation of Surface Latent Heat Flux Over the Ocean and its Relationship to Marine Atmospheric Boundary Layer (MABL) Structure
A new technique combining active and passive remote sensing instruments for the estimation of surface latent heat flux over the ocean is presented. This synergistic method uses aerosol lidar backscatter data, multi-channel infrared radiometer data and microwave scatterometer data acquired onboard the NASA P-3B research aircraft during an extended field campaign over the Atlantic ocean in support of the Lidar In-space Technology Experiment (LITE) in September of 1994. The 10 meter wind speed derived from the scatterometers and the lidar-radiometer inferred near-surface moisture are used to obtain an estimate of the surface flux of moisture via bulk aerodynamic formulae. The results are compared with the Special Sensor Microwave Imager (SSM/I) daily average latent heat flux and show reasonable agreement with an rms error and bias of about 50 and 25 W per square meters, respectively. In addition, the MABL height, entrainment zone thickness and integrated lidar backscatter intensity are computed from the lidar data and compared with the magnitude of the surface fluxes. The results show that the surface latent heat flux is most strongly correlated with entrainment zone top, bottom and the integrated MABL lidar backscatter, with corresponding correlation coefficients of 0.62, 0.67 and 0.61, respectively.
Palm, Stephen P.↗
Monolithic Arrays of Grating-Surface-Emitting Diode Lasers and Quantum Well Modulators for Optical Communications
The electro-optic switching properties of injection-coupled coherent 2-D grating-surface-emitting laser arrays with multiple gain sections and quantum well active layers are discussed and demonstrated. Within such an array of injection-coupled grating-surface-emitting lasers, a single gain section can be operated as intra-cavity saturable loss element that can modulate the output of the entire array. Experimental results demonstrate efficient sub-nanosecond switching of high power grading-surface-emitting laser arrays by using only one gain section as an intra-cavity loss modulator.
Carlson, N. W.↗
Hydrodynamic Modeling of Stratification and Mixing in a Shallow, Tropical Floodplain Lake
Abstract Floodplain lakes are widespread and ecologically important throughout tropical river systems, however data are rare that describe how temporal variations in hydrological, meteorological and optical conditions moderate stratification and mixing in these shallow lakes. Using time series measurements of meteorology and water‐column temperatures from 17 several day campaigns spanning two hydrological years in a representative Amazon floodplain lake, we calculated surface energy fluxes and thermal stratification, and applied and evaluated a 3‐dimensional hydrodynamic model. The model successfully simulated diel cycles in thermal structure characterized by buoyancy frequency, depth of the actively mixing layer, and other terms associated with the surface energy budget. Diurnal heating with strong stratification and nocturnal mixing were common; despite considerable heat loss at night, the strong stratification during the day meant that mixing only infrequently extended to the bottom at night. Simulations indicated that the diurnal thermocline up and downwelled creating lake‐wide differences in near‐surface temperatures and mixing depths. Infrequent full mixing creates conditions conducive to anoxia in these shallow lakes given their warm temperatures.
Environmental Sciences & Ecology↗
Orientation matters: Measuring the correct surface of polyamide membranes with quartz crystal microbalance
The surface of polyamide reverse osmosis (RO) membranes which regulates interface-dominated phenomena, such as partitioning and fouling, is the one facing the feed during operation. However, the opposite surface of the polyamide selective layer, the one facing the permeate and in contact with the polysulfone porous support, is commonly analyzed in quartz crystal microbalance (QCM) measurements due to limitations of state-of-the-art transfer methodologies. Such measurements on the back surface cannot be generalized because the polyamide layer is chemically and morphologically asymmetric. Herein, we introduce a simple method to coat QCM sensors with polyamide active layers in the correct orientation (i.e., exposing their front surface) and show that interface-dominated phenomena differ significantly between orientations. We start by describing a transfer protocol to coat any surface with a polyamide layer on its front surface orientation. We then systematically analyze the chemical and morphological differences between the two surfaces of the polyamide layer of a commercial RO membrane. Finally, we demonstrate that interface-dominated phenomena depend on the orientation by showing that NaCl partitioning at pH 6 was 1.3 to 2.3-fold higher on the front surface and that organic fouling with humic acid occurred at a lower rate on this surface. The new method presented herein enables measurements on the front surface of polyamide RO membranes, which should be the standard in any future QCM studies.
Fouling behavior↗
Membrane‐electrode assembly design parameters for optimal CO 2 reduction
Commercial-scale generation of carbon-containing chemicals and fuels by means of electrochemical CO 2 reduction (CO 2 R) requires electrolyzers operating at high current densities and product selectivities. Membrane-electrode assemblies (MEAs) have been shown to be suitable for this purpose. In such devices, the cathode catalyst layer controls both the rate of CO 2 R and the distribution of products. In this study, we investigate how the ionomer-to-catalyst ratio (I:Cat), catalyst loading, and catalyst-layer thickness influence the performance of a cathode catalyst layer containing Ag nanoparticles supported on carbon. In this paper, we explore how these parameters affect the cell performance and establish the role of the exchange solution (water vs. CsHCO 3 ) behind the anode catalyst layer in cell performance. We show that a high total current density is best achieved using an I:Cat ratio of 3 at a Ag loading of 0.01–0.1 mg Ag /cm 2 and with a 1.0 M solution of CsHCO 3 circulated behind the anode catalyst layer. For these conditions, the optimal CO partial current density depends on the voltage applied to the MEA. The work also reveals that the performance of the cathode catalyst layer is limited by a combination of the electrochemically active surface area and the degree to which mass transfer of CO 2 to the surface of the Ag nanoparticles and the transport of OH – anions away from it limit the overall catalyst activity. Hydration of the ionomer in the cathode catalyst layer is found not to be an issue when using an exchange solution. The insights gained allowed for a Ag CO 2 R MEA that operates between 200 mA/cm 2 and 1 A/cm 2 with CO faradaic efficiencies of 78–91%, and the findings and understanding gained herein should be applicable to a broad range of CO 2 R MEA-based devices.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Isolating the Electrocatalytic Activity of a Confined NiFe Motif within Zirconium Phosphate
Unique classes of active-site motifs are needed for improved electrocatalysis. Herein, the activity of a new catalyst motif is engineered and isolated for the oxygen evolution reaction (OER) created by nickel–iron transition metal electrocatalysts confined within a layered zirconium phosphate matrix. It is found that with optimal intercalation, confined NiFe catalysts have an order of magnitude improved mass activity compared to more conventional surface-adsorbed systems in 0.1 m KOH. Interestingly, the confined environments within the layered structure also stabilize Fe-rich compositions (90%) with exceptional mass activity compared to known Fe-rich OER catalysts. Through controls and by grafting inert molecules to the outer surface, it is evidenced that the intercalated Ni/Fe species stay within the interlayer during catalysis and serve as the active site. After determining a possible structure (wycherproofite), density functional theory is shown to correlate with the observed experimental compositional trends. It is further demonstrated that the improved activity of this motif is correlated to the Fe and water content/composition within the confined space. This work highlights the catalytic enhancement possibilities available through zirconium phosphate and isolates the activity from the intercalated species versus surface/edge ones, thus opening new avenues to develop and understand catalysts within unique nanoscale chemical environments.
36 MATERIALS SCIENCE↗
One-Step Synthesis and Operando Electrochemical Impedance Spectroscopic Characterization of Heterostructured MoP–Mo 2 N Electrocatalysts for Stable Hydrogen Evolution Reaction
Here this study presents a novel synthesis of self-standing MoP and Mo 2 N heterostructured electrocatalysts with enhanced stability and catalytic performance. Facilitated by the controlled phase and interfacial microstructure, the seamless structures of these catalysts minimize internal resistivity and prevent local corrosion, contributing to increased stability. The chemical synthesis proceeds with etching step to activate the surface, followed by phosphor-nitriding in a chemical vapor deposition chamber to produce MoP-Mo 2 N@Mo heterostructured electrocatalysts. X-ray diffraction analyses confirm the presence of MoP, Mo 2 N, and Mo phases in the electrocatalyst. Morphology studies using scanning electron microscopy characterizes the hierarchical growth of structures, indicating successful formation of the heterostructure. X-ray photoelectron spectroscopy (XPS) analyses of the as-synthesized and post-catalytic activity samples reveal the chemical shift in terms of binding energy (BE) of Mo 3d XPS peak, especially after catalytic activity. The XPS BE shifts attributed to changes in oxidation state, electron transfer, and surface reconstruction during catalysis. Electrochemical evaluation of the catalysts demonstrates the superior performance of the MoP-Mo 2 N@Mo heterostructured catalyst in hydrogen evolution reactions (HER), with lower overpotentials and enhanced Tafel slopes. Stability tests reveal changes in double layer capacitance over time, suggesting surface reconstruction and increased active surface area during catalysis. Operando electrochemical impedance spectroscopy (EIS) further elucidates the dynamic changes in resistance and charge transfer during HER. Overall, comprehensive understanding of the synthesis, characterization, and electrochemical behavior of the developed MoP-Mo 2 N@Mo heterostructured electrocatalyst as presented in this paper highlights their potential utilization in sustainable energy applications.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Microstructure and in-service degradation of baffle former bolts – in-core components of light water reactors
This report presents a microstructure evaluation of the baffle former bolt, a commercial pressurized water reactor component. Using SEM, EDS, and EBSD analysis the material was identified as AISI 316 steel with an annealed austenite microstructure. Findings include abnormal grain growth in a fraction of the grains and the absence of retained ferrite. Notable observations include an overlapping of pre- and post-irradiation deformation, including defect-free channel formation as an active deformation mechanism in the near-surface layer of BFB. Specimen surfaces, exposed to high-temperature, high-pressure water, exhibited signs of in-service corrosion degradation. EBSD and EDS analyses highlighted intergranular corrosion, possible grain boundary oxidation with depths less than 3 µm, and, unexpectedly, short cracks filled with Cr-rich oxides measuring around 5-6 µm. The presence of defect-free channels from EBSD data suggests episodes of high mechanical stresses during service. The specimens provide a potentially unique insight into the in-service degradation of NPP components, strain localization, and crack initiation processes. An intact corrosion layer reveals a complex component's in-service history. Further research is underway for a detailed analysis.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
Cosmic-ray exposure ages of the ordinary chondrites and their significance for parent body stratigraphy
Improved exposure ages are derived for 201 H, 203 L, and 38 LL chondrites in an effort to understand the characteristics of the chondrite parent body. The Ne-21 exposure ages were calculated from literature values taking into account shielding differences, a trapped component and radiogenic He. The exposure age distributions show clear peaks at 4.5 and 20 million years for the H chondrites, while the Ls and LLs appear more as a continuous series of intermediate peaks which may be modeled by at least six peaks between 1 and 35 million years in the case of L chondrites. The observations that every petrological type occurs in each large peak and contain solar wind gases suggest that the parent bodies have been fragmented and reassembled into a megabreccia. The H meteorites are proposed to represent the surface layer of a body with a substantial, active regolith as indicated by the relatively high abundances of solar gases. The L chondrites, on the other hand, are attributed to a parent body that was fragmented by collision about 500 million years ago.
Crabb, J.↗
Composite battery separator
A composite battery separator comprises a support element (10) having an open pore structure such as a ribbed lattice and at least one liquid permeable sheet (20,22) to distribute the compressive force evenly onto the surfaces of the layers (24, 26) of negative active material and positive active material. In a non-flooded battery cell the compressible, porous material (18), such as a glass mat which absorbs the electrolyte, is compressed into a major portion of the pores or openings (16) in the support element. The unfilled pores in the material (18) form a gas diffusion path as the channels (41) formed between adjacent ribs in the lattice element (30,36). Facing two lattice elements (30, 31) with acute angled cross-ribs (34, 38) facing each other prevents the elements from interlocking and distorting a porous, separator (42) disposed between the lattice elements.
Edwards, Dean B.↗
High Sensitivity Stress Sensor Based on Hybrid Materials
A sensing device is used to detect the spatial distributions of stresses applied by physical contact with the surface of the sensor or induced by pressure, temperature gradients, and surface absorption. The sensor comprises a hybrid active layer that includes luminophores doped in a polymeric or organic host, altogether embedded in a matrix. Under an electrical bias, the sensor simultaneously converts stresses into electrical and optical signals. Among many applications, the device may be used for tactile sensing and biometric imaging.
Cao, Xian-An↗
Laser Crystallization and Dopant Activation of a-Si:H Carrier-Selective Layer in TOPCon Si Solar Cells
Herein, we present a pulsed-laser processing method for crystallization and dopant activation of a highly n-doped amorphous silicon (a-Si:H) carrier-selective layer in a tunnel oxide passivated contact (TOPCon) Si solar cell structure. Here, the laser method provides enhanced conductivity and implied open circuit voltage while reducing emitter saturation current density and surface heating, as opposed to conventional high-temperature furnace annealing of the bulk Si wafer with a TOPCon structure. We identify an appropriate laser wavelength, fluence, and layer thickness using modeling and simulations. Raman and Hall effect measurements demonstrate increased crystallinity and dopant activation, whereas photoconductive decay shows enhanced surface and interface passivation quality. Additionally, we examine the role of subsequent SiNx deposition on further improving the passivation of laser-processed TOPCon layers to achieve a 5.9 kΩ/sq film sheet resistance, 2 ms effective carrier lifetime, 718 mV implied open-circuit voltage (iVOC), and 8.6 fA/cm 2 one-side recombination current density (J0) with the potential for further passivation improvement via laser process and a-Si layer thickness optimization.
14 SOLAR ENERGY↗