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Twinning Enhances Efficiencies of Metallic Catalysts toward Electrolytic Water Splitting
Twinning is demonstrated to be an effective way of enhancing efficiencies of metallic catalysts toward electrolytic water splitting. Dendritic Cu possessing dense coherent nanotwin (NT) boundaries (NTCu-5nm) is successfully prepared with an organic-assisted electrodeposition at high pulse current densities. NT boundaries significantly improve electrocatalytic efficiencies and stability of NTCu-5nm over nanocrystalline Cu (NCCu), reducing overpotentials at 10 mA cm -2 for the oxygen evolution reaction (OER) from 378 to 281 mV and from 235 to 88 mV for the hydrogen evolution reaction (HER), with a small chronoamperometric decay of 5% after 100 h continuous overall water splitting at an ultrahigh initial current density of 500 mA cm -2 , largely outperforming the large chronoamperometric decay of 27% for only 1 h operation of the NCCu//NCCu couple. The defective twin boundaries enable formation of active Cu III O 2 - at low overpotentials, thus enhancing OER performance. Furthermore, the synergistic geometric and electronic effects induced by the twin boundaries result in shifts in Gibbs free energies of hydrogen adsorption (ΔG H ) toward the apex of a volcano plot of exchange current density versus ΔG H , leading to the remarkable improvement in HER activity.
Scaling microstructural processes in the sintering of ionic ceramics
A multi-scale framework, combining a multiphase field formulation and large deformation mechanics, was developed as a stepping stone to perform the data analytics of the microstructural level kinetics of a sintering solid. Relevant microstructural information from this framework, such as grain, stress, and porosity statistics, was scaled up to describe the macroscopic level sintering kinetics. Here, the developed formulation was applied to describe the electric field assisted sintering of Y 2 O 3 . Microstructural inhomogeneities in a multi-granular solid result in the formation of a field of compressive stress networks, which interleave with low compression and weakly tensile regions, defining a scaffolding for sintering concentration regions to develop. A Poisson effect-induced lateral stress network is also naturally self-induced as a result of the mechanical constraints imposed by the sintering apparatus. For long sintering times, localized shear stresses enhancing mass flow along grain boundaries and internal surfaces develop. Three-sided pores are removed by either vacancy transport to the surrounding pores, or move towards the external surfaces through grain boundary diffusion. Four- and higher order-sided pores stabilize because an equal amount of vacancies are gained and lost through the connecting grain boundaries. Grain dewetting contributes to pore coalescence, suggesting that pore kinetics and grain growth are coupled and should be analyzed in concert. The combined sintering and grain growth kinetics define six regimes of sintering behavior: (1) T, the transient regime; (2) E$_Υ$, the surface energy dominated, early sintering regime, where the grain growth exponent, p = 1, and the stress concentration factor, $f$ ~ $1/\hat{ρ}^{4.6}$; (3) E S , the stress dominated, early sintering regime, where p = 1 and $f$ ~ $1/\hat{ρ}^{4}$; (4) I$_Υ$, the surface energy dominated, intermediate sintering regime, where p = 2 and $f$ ~ $1/\hat{ρ}^{4.6}$; (5) I S , the stress dominated, intermediate sintering regime, where p = 2 and $f$ ~ $1/\hat{ρ}^{4}$; and (6) L, the late sintering regime, where p = 3 and $f$ ~ 1. At the macroscopic level, the rapid densification and suppression of grain growth observed in the electric field assisted sintering process is a consequence of the compounding effects of the underlying stress-, transport-, and interfacial-energy-induced energy minimization kinetics, as predicted by the multi-scale framework.
Laboratory studies of baroclinic instability at small Richardson number
As part of the support program for the Atmospheric General Circulation Experiment, laboratory studies of baroclinic and other convective instabilities were performed for a thin layer of fluid between thermally conducting horizontal discs. There were three types of modes identified. The first has a spiral-arm appearance, and exists for large enough horizontal thermal forcing, weak enough static stability, and large enough rotation. The source of this wave is shown to be the Eady mode of instability. The second mode is due to convective instability in the thermal boundary layers which exist due to the thermally conducting horizontal boundaries. Finally, for strong enough negative static stability, thermal convection of the Benard type appears. The most significant result is that the symmetric (Solberg) mode was not found, even though the infinite-plane theory predicts this mode under certain experimental conditions.
A strain-driven thermotropic phase boundary in BaTiO 3 at room temperature by cycling compression
In BaTiO 3 single crystals, we observed a strain-driven phase transition from the tetragonal phase to the tetragonal-orthorhombic phase boundary which can be introduced by slow cycling compressions (a loading of up to 0.5 GPa, strain rate of 10 -4 s -1 , and 100 cycles) at room temperature. Different from the well-known tetragonal to cubic phase transition under stress (~2 GPa), it only takes place locally around bent 90° domain walls. The inhomogeneous local stress and electrical fields as well as the mobile point defect pinning effect contribute to the phase re-entrance. Through comparison experiments by in situ synchrotron x-ray diffraction, Raman scattering, and (scanning) transmission electron microscopy, we explored the phase transition mechanism. Based on that, we developed a mechanical method to obtain well-stabilized high-density thermotropic phase boundary structures (with tetragonal, orthorhombic, and bridging monoclinic phases) in BaTiO 3 for potential applications.
The second-generation Shifted Boundary Method and its numerical analysis
Recently, the Shifted Boundary Method (SBM) was proposed within the class of unfitted (or immersed, or embedded) finite element methods. By reformulating the original boundary value problem over a surrogate (approximate) computational domain, the SBM avoids integration over cut cells and the associated problematic issues regarding numerical stability and matrix conditioning. Accuracy is maintained by modifying the original boundary conditions using Taylor expansions. Hence the name of the method, that shifts the location and values of the boundary conditions. In this article, we present enhanced variational SBM formulations for the Poisson and Stokes problems with improved flexibility and robustness. These simplified variational forms allow to relax some of the assumptions required by the mathematical proofs of stability and convergence of earlier implementations. First, we show that these new SBM implementations can be proved asymptotically stable and convergent even without the rather restrictive assumption that the inner product between the normals to the true and surrogate boundaries is positive. Second, we show that it is not necessary to introduce a stabilization term involving the tangential derivatives of the solution at Dirichlet boundaries, therefore avoiding the calibration of an additional stabilization parameter. Finally, we prove enhanced L 2 -estimates without the cumbersome assumption – of earlier proofs – that the surrogate domain is convex. Instead we rely on a conventional assumption that the boundary of the true domain is smooth, which can also be replaced by requiring convexity of the true domain. The aforementioned improvements open the way to a more general and efficient implementation of the Shifted Boundary Method, particularly in complex three-dimensional geometries. We complement these theoretical developments with numerical experiments in two and three dimensions.
On the instability of a three-dimensional attachment-line boundary layer - Weakly nonlinear theory and a numerical approach
The instability of a three-dimensional attachment-line boundary layer is considered in the nonlinear regime. Using weakly nonlinear theory, it is found that, apart from a small interval near the (linear) critical Reynolds number, finite-amplitude solutions bifurcate subcritically from the upper branch of the neutral curve. The time-dependent Navier-Stokes equations for the attachment-line flow have been solved using a Fourier-Chebyshev spectral method and the subcritical instability is found at wavenumbers that correspond to the upper branch. Both the theory and the numerical calculations show the existence of supercritical finite-amplitude (equilibrium) states near the lower branch which explains why the observed flow exhibits a preference for the lower branch modes. The effect of blowing and suction on nonlinear stability of the attachment-line boundary layer is also investigated.
Preliminary Analysis of the Effect of Flow Separation Due to Rocket Jet Pluming on Aircraft Dynamic Stability During Atmospheric Exit
A theoretical investigation was conducted to determine the effects of body boundary-layer separation resulting from a highly underexpanded jet on the dynamic stability of a typical rocket aircraft during an atmospheric exit trajectory. The particular flight condition studied on a digital computer for five degrees of freedom was at Mach 6.0 and 150,000 feet. In view of the unknown character of the separated flow field, two estimates of the pressures in the separated region were made to calculate the unbalanced forces and moments. These estimates, based on limited fundamental zero-angle-of-attack studies and observations, are believed to cover what may be the actual case. In addition to a fixed control case, two simulated pilot control inputs were studied: rate-limited and instantaneous responses. The resulting-motions with and without boundary-layer separation were compared for various initial conditions. The lower of the assumed misalinement forces and moments led to a situation whereby a slowly damped motion could be satisfactorily controlled with rate-limited control input. The higher assumption led to larger amplitude, divergent motions when the same control rates were used. These motions were damped only when the instantaneous control responses were assumed.
Unraveling Grain Boundary Instability in Dense Proton-Conducting Oxides
The long-term stability of protonic ceramic electrolysis cell (PCEC) materials under high-steam operating conditions remains a critical barrier to device commercialization. Here, we investigate the fundamental degradation mechanisms of dense BaCe 0.7 Zr 0.1 Y 0.1 Yb 0.1 O 3-δ (BCZYYb) electrolytes operated at 550 °C, 50% H 2 O in air. Over 1,000 h, the total electrolyte conductivity decreases by 11.1%, driven primarily by a >130% increase in grain-boundary resistivity. Post-mortem analyses reveal that damage is localized to near-surface grain boundaries extending ∼50 μm into the dense electrolyte pellet. This surface localization indicates that degradation is likely to be severe in thin, device-level electrolytes. Degradation is primarily attributed to chemo-mechanical grain-boundary weakening arising from hydration-induced chemical expansion, culminating in the formation of intergranular cracks oriented parallel to the pellet surface. These internal cracks subsequently react with steam and/or CO 2 , leading to the formation of nanoscale insulating phases, including Ba(OH) 2 , nanocrystalline BaCO 3 , and amorphous Ce/Zr/Y/Yb-containing oxides or hydroxycarbonates. After an initial degradation period of approximately 200 h, the overall conductivity stabilizes. Incorporating NiO sintering aids reduces grain-boundary density by an order of magnitude under identical sintering conditions. Although addition of NiO increases the initial resistivity by >160% at 550 °C, it substantially suppresses grain-boundary instability and mitigates chemical degradation. These findings underscore the urgent need for chemical and/or physical stabilization of BCZYYb electrolytes and offer design guidelines to enable durable, high-performance PCECs.
Stable boundary approximations for a class of implicit schemes for the one-dimensional inviscid equations of gas dynamics
The applicability to practical calculations of recent theoretical developments in the stability analysis of difference approximations for initial-boundary-value problems of the hyperbolic type. For the numerical experiments, select the one-dimensional inviscid gas-dynamic equations in conservation-law form is selected. A class of implicit schemes based on linear multistep methods for ordinary differential equations is chosen and the use of space or space-time extrapolations as implicit or explicit boundary schemes is emphasized. Some numerical examples with various inflow-outflow conditions highlight the commonly discussed issues: explicit versus implicit boundary schemes, unconditionally stable schemes, and underspecification or overspecification of boundary conditions.
Investigating the physical mechanisms that modify wind plant blockage in stable boundary layers
Abstract. Wind plants slow down the approaching wind, a phenomenon known as blockage. Wind plant blockage undermines turbine performance for front-row turbines and potentially for turbines deeper into the array. We use large-eddy simulations to characterize blockage upstream of a finite-size wind plant in flat terrain for different atmospheric stability conditions and investigate the physical mechanisms modifying the flow upstream of the turbines. To examine the influence of atmospheric stability, we compare simulations of two stably stratified boundary layers using the Weather Research and Forecasting model in large-eddy simulation mode, representing wind turbines using the generalized actuator disk approach. For a wind plant, a faster cooling rate at the surface, which produces stronger stably stratified flow in the boundary layer, amplifies blockage. As a novelty, we investigate the physical mechanisms amplifying blockage by evaluating the different terms in the momentum conservation equation within the turbine rotor layer. The velocity deceleration upstream of a wind plant is caused by an adverse pressure gradient and momentum advection out of the turbine rotor layer. The cumulative deceleration of the flow upstream of the front-row turbines instigates vertical motions. The horizontal flow is diverted vertically, reducing momentum availability in the turbine rotor layer. Although the adverse pressure gradient upstream of the wind plant remains unchanged with atmospheric stability, vertical advection of horizontal momentum is amplified in the more strongly stable boundary layer, mainly by larger shear of the horizontal velocity, thus increasing the blockage effect.
Measurements in a Transitioning Cone Boundary Layer at Freestream Mach 3.5
An experimental study was conducted in the Supersonic Low-Disturbance Tunnel to investigate naturally-occurring instabilities in a supersonic boundary layer on a 7 deg half- angle cone. All tests were conducted with a nominal freestream Mach number of M(sub infinity) = 3:5, total temperature of T(sub 0) = 299:8 K, and unit Reynolds numbers of Re(sub infinity) x 10(exp -6) = 9:89, 13.85, 21.77, and 25.73 m(exp -1). Instability measurements were acquired under noisy- ow and quiet- ow conditions. Measurements were made to document the freestream and the boundary-layer edge environment, to document the cone baseline flow, and to establish the stability characteristics of the transitioning flow. Pitot pressure and hot-wire boundary- layer measurements were obtained using a model-integrated traverse system. All hot- wire results were single-point measurements and were acquired with a sensor calibrated to mass ux. For the noisy-flow conditions, excellent agreement for the growth rates and mode shapes was achieved between the measured results and linear stability theory (LST). The corresponding N factor at transition from LST is N 3:9. The stability measurements for the quiet-flow conditions were limited to the aft end of the cone. The most unstable first-mode instabilities as predicted by LST were successfully measured, but this unstable first mode was not the dominant instability measured in the boundary layer. Instead, the dominant instabilities were found to be the less-amplified, low-frequency disturbances predicted by linear stability theory, and these instabilities grew according to linear theory. These low-frequency unstable disturbances were initiated by freestream acoustic disturbances through a receptivity process that is believed to occur near the branch I locations of the cone. Under quiet-flow conditions, the boundary layer remained laminar up to the last measurement station for the largest Re1, implying a transition N factor of N greater than 8:5.
Role of thermo-mechanical gyrations on the α/β interface stability in a Ti6Al4V AM alloy
Fluctuating energy distributions experienced during Additive Manufacturing yield an evolution of spatial and temporal transients within a part. In general, the in-situ monitoring of these transients is near to impossible during manufacturing. In order to then gain perspective into the impact on these localized thermo-mechanical transients on the interface stability, rapid thermo-mechanical reversals with known boundary conditions are imposed on an AM Ti6Al4V alloy which resulted in a phase transformation leading to an increased β phase stability. Our goal with this study is to comprehend the kinetics of this phase transformation with concepts of stored energy due to plastic strain accumulation and diffusion kinetics. Atom Probe Tomography is employed to study the partitioning of the solute elements across the interface. As expected, the thermo-mechanically cycled samples showed a reduced Vanadium concentration across the β phase. Finally, this concentration profile across the interface, alongside a full-width-half-max analysis, provided insight on the potential phase transformation kinetics involved in the α → β transformation subject to thermo- mechanical gyrations.
Base Pressure at Supersonic Speeds on Two-dimensional Airfoils and on Bodies of Revolution with and Without Fins Having Turbulent Boundary Layers
An analysis has been made of available experimental data to show the effects of most of the variables that are more predominant in determining base pressure at supersonic speeds. The analysis covers base pressures for two-dimensional airfoils and for bodies of revolution with and without stabilizing fins and is restricted to turbulent boundary layers. The present status of available experimental information is summarized as are the existing methods for predicting base pressure. A simple semiempirical method is presented for estimating base pressure. For two-dimensional bases, this method stems from an analogy established between the base-pressure phenomena and the peak pressure rise associated with the separation of the boundary layer. An analysis made for axially symmetric flow indicates that the base pressure for bodies of revolution is subject to the same analogy. Based upon the methods presented, estimations are made of such effects as Mach number, angle of attack, boattailing, fineness ratio, and fins. These estimations give fair predictions of experimental results. (author)
Laminar to Turbulence Transition in Boundary Layers due to Tripping Devices
Direct numerical simulations (DNS)and linear stability analyses were performed to identify the mechanisms by whichtwo-and three-dimensional trips promote early transition in subsonic boundary layers over a flat plate. Investigations were conducted for threeboundary-layer transition trip configurations:a two-dimensional smooth hump,a two-dimensional rectangular-shapedrod and a three-dimensional zig-zagtape. The smooth hump was used by Park et al.1in the linear and nonlinear parabolized stability (PSE) computations. Reynolds numbersbased on the tripheights are 710, 683,and 300 for the two-and three-dimensional trips, respectively. Simulations withthe smooth hump showed that the flow becomes stable upstream and strongly unstable downstream of the hump. Simulations with the two-dimensional rectangular trip showed that the flow separates at the top of the trip and forms a long recirculation zonedownstream. However, the flow remains steady in the simulation without any external disturbances. Linear stability analysis showed that the inflectional profile in the recirculation zone is strongly unstable to frequencies in the range of 100-300 Hz. Simulations with the external disturbances forced at the frequency of 200 Hz showed that disturbances grow strongly inside the recirculation zone as observed in the Klebanoff2 experiment. Three-dimensional simulations with secondary disturbances of fundamental, subharmonic, and oblique types produced turbulent flows shortlydownstream. The three-dimensional zig-zag trip with a small roughness Reynolds number lead to early breakdown to a turbulent flow.
Viscous drag reduction in boundary layers
The present volume discusses the development status of stability theory for laminar flow control design, applied aspects of laminar-flow technology, transition delays using compliant walls, the application of CFD to skin friction drag-reduction, active-wave control of boundary-layer transitions, and such passive turbulent-drag reduction methods as outer-layer manipulators and complex-curvature concepts. Also treated are such active turbulent drag-reduction technique applications as those pertinent to MHD flow drag reduction, as well as drag reduction in liquid boundary layers by gas injection, drag reduction by means of polymers and surfactants, drag reduction by particle addition, viscous drag reduction via surface mass injection, and interactive wall-turbulence control.
Effect of Far-Field Boundary Conditions on Boundary-Layer Transition
The effect of far-field boundary conditions on the evolution of a finite-amplitude two-dimensional wave in the Blasius boundary layer is assessed. With the use of the parabolized stability equations (PSE) theory for the numerical computations, either asymptotic, Dirichlet, Neumann or mixed boundary conditions are imposed at various distances from the wall. The results indicate that asymptotic and mixed boundary conditions yield the most accurate mean-flow distortion and unsteady instability modes in comparison with the results obtained with either Dirichlet or Neumann conditions.
Effect of Far-Field Boundary Conditions on Boundary-Layer Transition
The effect of far-field boundary conditions on the evolution of a finite-amplitude two-dimensional wave in the Blasius boundary layer is assessed. With the use of the parabolized stability equations (PSE) theory for the numerical computations, either asymptotic, Dirichlet, Neumann or mixed boundary conditions are imposed at various distances from the wall. The results indicate that asymptotic and mixed boundary conditions yield the most accurate mean-flow distortion and unsteady instability modes in comparison with the results obtained with either Dirichlet or Neumann conditions.