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At least 577 records · Page 32

Mesoscopic analyses of the impact of morphology and operating conditions on the transport resistances in a proton-exchange-membrane fuel-cell catalyst layer

Exploring the origins of local transport resistance and characterizing the oxygen transport resistances in the catalyst layer (RCL) are critical for cost reduction. In this paper, a comprehensive mesoscopic model for simulating coupled transport processes of oxygen and water vapor for different structural parameters under different operating conditions in reconstructed microstructures is proposed. The local transport resistance is calculated after achieving the limiting current density and the effective diffusivity of oxygen. The results demonstrate that RCL increases greatly with decreasing platinum loading (LPt) and the transport resistances in other components of the cell dominate for high-loadings. Both the reduced oxygen permeation coefficient in the ionomer thin-film and the adsorption resistance account for the origins of local transport resistance. The local transport resistance increases with the bare carbon ratio for a constant LPt and Pt/C ratio due to the decreased effective ionomer surface, and increases with the I/C ratio due to the increased ionomer thickness and decreased Knudsen diffusivity. Due to the presence of liquid water, a slight decrease followed by an increase of the local transport resistance versus relative humidity is obtained. The contribution of ionomer thin-films to RCL is more sensitive to liquid saturation compared with that of pores. This journal is

Mu, YT↗

Precision surface modification of solid oxide fuel cells via layer-by-layer surface sol–gel deposition

While solid oxide fuel cells (SOFCs) are a promising technology for a clean and sustainable future, their commercialization is hindered by limited durability and performance. Here, we report our findings on the application of a layer-by-layer surface sol–gel (SSG) coating of catalysts to dramatically enhance the electro-catalytic activity and durability of SOFC cathodes. The SSG process is capable of penetrating and preserving complex backbone microstructures of porous electrodes, creating highly conformal coatings of controlled morphology, while tailoring the composition of the surface to improve catalytic properties and durability. For example, the application of an SSG coating of PrO x to a La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3–δ (LSCF) cathode has reduced the polarization resistance from 1.136 to 0.117 Ω cm 2 at 600 °C and the degradation rate from 1.13 × 10 –3 to 2.67 × 10 –4 Ω cm 2 h –1 at 650 °C. In addition, a continuous improvement in electrode performance is demonstrated as the thickness of the coating is increased, corresponding to the linear addition of catalyst. Furthermore, this first application of the SSG technique to SOFC systems opens the door for the controlled surface modification of porous components in electrochemical systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electromagnetic instability of thin reconnection layers: Comparison of three-dimensional simulations with MRX observations

In this study, the influence of current-aligned instabilities on magnetic reconnection in weakly collisional regimes is investigated using experimental observations from Magnetic Reconnection Experiment (MRX) [M. Yamada et al., Phys. Plasmas 4, 1936 (1997)] and large-scale fully kinetic simulations. In the simulations as well as in the experiment, the dominant instability is localized near the center of the reconnection layer, produces large perturbations of the magnetic field, and is characterized by the wavenumber that is a geometric mean between electron and ion gyroradii k~(ρ e ρ i ) -1/2 . However, both the simulations and the experimental observations suggest the instability is not the dominant reconnection mechanism under parameters typical of MRX.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Tunneling spectroscopy of superconducting MoN and NbTiN grown by atomic layer deposition

A tunneling spectroscopy study is presented of superconducting MoN and Nb{sub 0.8}Ti{sub 0.2}N thin films grown by atomic layer deposition (ALD). The films exhibited a superconducting gap of 2 meV and 2.4 meV, respectively, with a corresponding critical temperature of 11.5 K and 13.4 K, among the highest reported T{sub c} values achieved by the ALD technique. Tunnel junctions were obtained using a mechanical contact method with a Au tip. While the native oxides of these films provided poor tunnel barriers, high quality tunnel junctions with low zero bias conductance (below ∼10%) were obtained using an artificial tunnel barrier of Al{sub 2}O{sub 3} on the film's surface grown ex situ by ALD. We find a large critical current density on the order of 4 × 10{sup 6} A/cm{sup 2} at T = 0.8T{sub c} for a 60 nm MoN film and demonstrate conformal coating capabilities of ALD onto high aspect ratio geometries. These results suggest that the ALD technique offers significant promise for thin film superconducting device applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Direct atomic-scale observation of layer-by-layer oxide growth during magnesium oxidation

The atomic-scale oxide growth dynamics are directly revealed by in situ high resolution transmission electron microscopy during the oxidation of Mg surface. The oxidation process is characterized by the layer-by-layer growth of magnesium oxide (MgO) nanocrystal via the adatom process. Consistently, the nucleated MgO crystals exhibit faceted surface morphology as enclosed by (200) lattice planes. It is believed that the relatively lower surface energies of (200) lattice planes should play important roles, governing the growth mechanism. These results facilitate the understanding of the nanoscale oxide growth mechanism that will have an important impact on the development of magnesium or magnesium alloys with improved resistance to oxidation.

36 MATERIALS SCIENCE↗

Catalyst synthesis and evaluation using an integrated atomic layer deposition synthesis–catalysis testing tool

An integrated atomic layer deposition-catalysis (I-ALD-CAT) tool was developed, combining an ALD manifold with a plug-flow reactor system for the synthesis of supported catalytic materials by ALD and immediate evaluation of catalyst reactivity using gas-phase probe reactions. The I-ALD-CAT system can deliver gaseous reagents comprised of 12 different metal ALD precursors, 4 oxidizing or reducing agents, and 4 catalytic reaction feeds to either of the two plug-flow reactors. The system can employ reactor pressures and temperatures in the range of 10 -3 to 1 bar and 300–1000 K, respectively. Furthermore, the instrument is also equipped with a gas chromatograph and a mass spectrometer unit for the detection and quantification of volatile species from ALD and catalytic reactions. In this report, we demonstrate the use of the I-ALD-CAT tool for the ALD of platinum active sites and Al 2 O 3 overcoats, and evaluation of catalyst propylene hydrogenation activity.

47 OTHER INSTRUMENTATION↗

Impact of La{sub 2}O{sub 3} interfacial layers on InGaAs metal-oxide-semiconductor interface properties in Al{sub 2}O{sub 3}/La{sub 2}O{sub 3}/InGaAs gate stacks deposited by atomic-layer-deposition

We examine the electrical properties of atomic layer deposition (ALD) La{sub 2}O{sub 3}/InGaAs and Al{sub 2}O{sub 3}/La{sub 2}O{sub 3}/InGaAs metal-oxide-semiconductor (MOS) capacitors. It is found that the thick ALD La{sub 2}O{sub 3}/InGaAs interface provides low interface state density (D{sub it}) with the minimum value of ∼3 × 10{sup 11} cm{sup −2} eV{sup −1}, which is attributable to the excellent La{sub 2}O{sub 3} passivation effect for InGaAs surfaces. It is observed, on the other hand, that there are a large amount of slow traps and border traps in La{sub 2}O{sub 3}. In order to simultaneously satisfy low D{sub it} and small hysteresis, the effectiveness of Al{sub 2}O{sub 3}/La{sub 2}O{sub 3}/InGaAs gate stacks with ultrathin La{sub 2}O{sub 3} interfacial layers is in addition evaluated. The reduction of the La{sub 2}O{sub 3} thickness to 0.4 nm in Al{sub 2}O{sub 3}/La{sub 2}O{sub 3}/InGaAs gate stacks leads to the decrease in hysteresis. On the other hand, D{sub it} of the Al{sub 2}O{sub 3}/La{sub 2}O{sub 3}/InGaAs interfaces becomes higher than that of the La{sub 2}O{sub 3}/InGaAs ones, attributable to the diffusion of Al{sub 2}O{sub 3} through La{sub 2}O{sub 3} into InGaAs and resulting modification of the La{sub 2}O{sub 3}/InGaAs interface structure. As a result of the effective passivation effect of La{sub 2}O{sub 3} on InGaAs, however, the Al{sub 2}O{sub 3}/10 cycle (0.4 nm) La{sub 2}O{sub 3}/InGaAs gate stacks can realize still lower D{sub it} with maintaining small hysteresis and low leakage current than the conventional Al{sub 2}O{sub 3}/InGaAs MOS interfaces.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

First results of radiation-driven, layered deuterium-tritium implosions with a 3-shock adiabat-shaped drive at the National Ignition Facility

Radiation-driven, layered deuterium-tritium plastic capsule implosions were carried out using a new, 3-shock “adiabat-shaped” drive on the National Ignition Facility. The purpose of adiabat shaping is to use a stronger first shock, reducing hydrodynamic instability growth in the ablator. The shock can decay before reaching the deuterium-tritium fuel leaving it on a low adiabat and allowing higher fuel compression. The fuel areal density was improved by ~25% with this new drive compared to similar “high-foot” implosions, while neutron yield was improved by more than 4 times, compared to “low-foot” implosions driven at the same compression and implosion velocity.

42 ENGINEERING↗

The structure and properties of single-layer and gradient-layered coatings of the Ti–Al–Si–Cr–Mo–S–N system

Using the method of microprobe analysis and transmission electron microscopy, the influence of obtaining conditions upon particular elemental composition and growth structure coatings of Ti–Al–Si–Mo–S–N system was studied. The possibility of formation and characteristics of the structural and elastic-stress state single-layer coatings with nanoscale columnar or equiaxed grains and gradient-layered, combining two types of selected structure, was defined. On the basis of hardness, tribological properties and coating hardness, a conclusion was made about the relative prospects of its use as wear-resistant coatings with a nanocrystalline structure.

36 MATERIALS SCIENCE↗

Mechanism of hole injection enhancement in light-emitting diodes by inserting multiple hole-reservoir layers in electron blocking layer

In this study, gallium nitride (GaN) based light-emitting diodes (LEDs) with single and multiple hole-reservoir layers (HRLs) inserted in the electron-blocking layer (EBL) have been investigated numerically and experimentally. According to simulation results, a better electron confinement and a higher hole injection level can be achieved by the multiple HRLs inserted in the EBL region. To further reveal the underlying mechanism of hole injection enhancement experimentally, the active regions were intentionally designed to emit photons with three different wavelengths of 440 nm, 460 nm, and 480 nm, respectively. Based on the experimental results of photoluminescence (PL) and time-resolved PL (TRPL) measurements conducted at 298 K, the remarkable enhancement (148%) of PL intensities and significant increase in the decay times of the quantum wells close to p-GaN can be obtained. Therefore, the mechanism is proposed that carriers are able to reserve in the EBL region with multiple HRLs for a much longer time. Meanwhile, carriers could diffuse into the active region by tunnelling and/or thermo-electronic effect and then recombine efficiently, leading to the better carrier reservoir effect and higher hole injection in LEDs. As a result, by inserting multiple HRLs in the EBL region instead of single HRL, the experimental external quantum efficiency is enhanced by 19.8%, while the serious droop ratio is markedly suppressed from 37.0% to 27.6% at the high current injection of 100 A/cm{sup 2}.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Integrated modeling of cryogenic layered highfoot experiments at the NIF

Integrated radiation hydrodynamic modeling in two dimensions, including the hohlraum and capsule, of layered cryogenic HighFoot Deuterium-Tritium (DT) implosions on the NIF successfully predicts important data trends. The model consists of a semi-empirical fit to low mode asymmetries and radiation drive multipliers to match shock trajectories, one dimensional inflight radiography, and time of peak neutron production. Application of the model across the HighFoot shot series, over a range of powers, laser energies, laser wavelengths, and target thicknesses predicts the neutron yield to within a factor of two for most shots. The Deuterium-Deuterium ion temperatures and the DT down scattered ratios, ratio of (10–12)/(13–15) MeV neutrons, roughly agree with data at peak fuel velocities <340 km/s and deviate at higher peak velocities, potentially due to flows and neutron scattering differences stemming from 3D or capsule support tent effects. These calculations show a significant amount alpha heating, 1–2.5× for shots where the experimental yield is within a factor of two, which has been achieved by increasing the fuel kinetic energy. This level of alpha heating is consistent with a dynamic hot spot model that is matched to experimental data and as determined from scaling of the yield with peak fuel velocity. Lastly, these calculations also show that low mode asymmetries become more important as the fuel velocity is increased, and that improving these low mode asymmetries can result in an increase in the yield by a factor of several.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Evidence of Photo-induced Dynamic Competition of Metallic and Insulating Phase in a Layered Manganite.

We show evidence that the competition between the antiferromagetic metallic phase and the charge- and orbital-ordered insulating phase at the reentrant phase boundary of a layered manganite, LaSr2Mn2O7, can be manipulated using ultrafast optical excitation. The time- dependent evolution of the Jahn-Teller superlattice reflection, which indicates the formation of the charge and orbital order, was measured at different laser fluences. The laser-induced enhancement and reduction the Jahn-Teller reflection intensity shows a reversal of sign between earlier (~10 ns) and later (~150 ns) time delays during the relaxation after photo excitation. This effect is consistent with a scenario whereby the laser excitation modulates the local competition between the metallic and the insulating phases.

Li, Yuelin↗

Layer-by-layer assembly of a [Fe-(pyrazine){Pd(CN) 4 }] spin crossover thin film

Abstract [Fe-(pyrazine){Pd(CN) 4 }] (pyrazine = pz) thin films were fabricated using a layer-by-layer assembly approach, a method known to be tunable, versatile, and scalable, since thin films are better-suited for industrial applications. In this study, [Fe-(pz){Pd(CN) 4 }] powder was synthesized, and the results obtained from a vibrating sample magnetometer verified the presence of an abrupt hysteresis loop with widths of 45 K centered around 300 K, indicating good cooperativity. Super conducting quantum interference device magnetometry results indicated a slow spin transition with temperature but with evidence of hysteresis for thin film samples. X-ray absorption analysis provided further support of the spin crossover behavior but differs from the magnetometry because the spin state transition at the surface differs from the bulk of the thin film. X-ray photoelectron spectroscopy provided some insight into issues with the film deposition process and multiplex fitting was used to further support the claim that the surface of the film is different than the bulk of the film.

McElveen, Kayleigh A. (ORCID:0000000210302913)↗

Layer-by-layer assembly of metal-organic framework nanosheets with polymer

Metal-organic framework (MOF) nanosheets are gaining more and more attention due to their tunable porous structure and two-dimensional shape. Adding MOF nanosheets into polymers can lead to improved properties, but the level of enhancement is usually thwarted by the difficulties in exfoliating and aligning these nanosheets within the polymer matrix. In order to establish a strategy for making polymer/MOF nanosheets composites with improved exfoliation and alignment, we combined MOF nanosheets and polymer using layer-by-layer (LbL) assembly for the first time. MOF nanosheets (ZIF67-L, leaf-like zeolitic imidazolate framework nanosheets) used here were functionalized with positively charged polyethylenimine, which could replace the original surface ligands and impart a positive charge on the nanosheet surface. These positively charged MOF nanosheets were then combined with negatively charged poly(acrylic acid) through ionic-bonding-assisted LbL assembly, generating a polymer composite with fully exfoliated and highly aligned MOF nanosheets.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Ferrimagnetic spin waves in honeycomb and triangular layers of Mn{sub 3}Si{sub 2}Te{sub 6}.

A detailed analysis of the ferrimagnetic ground state of Mn 3 Si 2 Te 6 has been performed using inelastic neutron scattering. Although the proposed valence of the nominal Mn 2+ ions would have quenched orbital angular momentum, a significant exchange anisotropy exists in Mn 3 Si 2 Te 6 . This apparent exchange anisotropy is a manifestation of a weak spin-orbit coupling in the layered material. We employ a detailed simulation of the spin-wave spectrum coupling traditional refinement of dispersion parameters to image analysis techniques, while including Monte Carlo simulations of the instrumental resolution to accurately identify the exchange couplings to the third nearest neighbor. An independent validation of our results is made by comparing our final Hamiltonian to heat capacity measurements.

Sala, G.↗