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Constitutional under-potential plating (CUP) – New insights for predicting the morphological stability of deposited lithium anodes in lithium metal batteries
Lithium (Li) cycling in lithium metal batteries (LMBs) inevitably witnesses a non-planar Li/electrolyte interface (cellular/dendritic microstructure) affecting the performance, safety and reliability of LMBs. Herein, the “constitutional under-potential plating” (CUP) concept is presented for the first time to understand the evolution, formation and predict the morphological stability/instability of the Li/electrolyte interface. Here, the CUP condition, a measure of the driving force for interface perturbation, occurs when the true potential gradient at the interface is smaller than the equilibrium electrodeposition potential gradient at the Li/electrolyte interface resulting in the electrolyte ahead of the Li-electrolyte interface to be in an under-potential state. Detailed CUP criterion calculations conducted herein establishes the relationship of battery operating conditions (e.g. current density, potential gradient) with the electrolyte properties (e.g. Li-ion transference number and diffusion coefficient) predicting the morphological stability condition at the interface. In addition to the driving force for interface perturbation, the capillarity effect or the Gibbs Thomson effect, a measure of the resistance to perturbation of the perturbed interface is discussed for understanding the influence of interfacial energy/adhesion energy between the current collector and the deposited Li on the overall morphological stability of the Li/electrolyte interface, a critical criterion for the unwanted dendritic morphology.
USML-1 Glovebox experiments
This report covers the development of and results from three experiments that were flown in the Materials Science Glovebox on USML-1: Marangoni convection in Closed Containers (MCCC), Double Float Zone (DFZ), and Fiber Pulling in Microgravity (FPM). The Glovebox provided a convenient, low cost method for doing simple 'try and see' experiments that could test new concepts or elucidate microgravity phenomena. Since the Glovebox provided essentially one (or possibly two levels of confinement, many of the stringent verification and test requirements on the experiment apparatus could be relaxed and a streamlined test and verification plan for flight qualification could be implemented. Furthermore, the experiments were contained in their own carrying cases whose external configurations could be identified early in the integration sequence for stowage considerations while delivery of the actual experiment apparatus could be postponed until only a few months before flight. This minimized the time fluids must be contained and reduced the possibility of corrosive reactions that could ruin the experiment. In many respects, this exercise was as much about developing a simpler, cheaper way of doing crew-assisted science as it was about the actual scientific accomplishments of the individual experiments. The Marangoni Convection in Closed Containers experiment was designed to study the effects of a void space in a simulated Bridgman crystal growth configuration and to determine if surface tension driven convective flows that may result from thermal gradients along any free surfaces could affect the solidification process. The Fiber Pulling in Microgravity experiment sought to separate the role of gravity drainage from capillarity effects in the break-up of slender cylindrical liquid columns. The Stability of a Double Float Zone experiment explored the feasibility of a quasi-containerless process in which a solidifying material is suspended by two liquid bridges of its own melt.
Petaloid-shaped ZnO coated carbon felt as a controllable host to construct hierarchical Li composite anode
Prestoring Li metal into the 3D host via thermal infusion strategy has been considered as an effective approach on suppressing Li dendrites growth of Li-metal anode during cycling. However, the fast Li infusing process generally induces uncontrollable and undesirable structures during the formation of composite Li metal anode. It is widely accepted that both physical and chemical interactions between the molten Li and the hosts provide driving forces for Li infusing into the host, but which one plays the dominant role has not been explored clearly. In this work, a 3D carbon felt coated by petaloid zinc oxide (CFZO) is designed as a controllable host for prestoring Li metal via thermal infusion method. It is revealed that the morphology induced physical driving force plays a more important role than the chemical reaction between ZnO and molten Li in the thermal infusion process. The physical driving force originates from the capillarity effect, depending on the roughness of the host according to Wenzel's model. An adjustable Li infusing process can be controlled to fabricate the Li composite electrode with a hierarchical structure (with dense Li-rich layer and porous Li-poor layer). The unique structure of the CFZO-Li not only provides enough spaces for Li deposition, but also disperses local current density to induce a uniform Li deposition behavior, thus Li dendrites can be suppressed effectively. As a result, CFZO-Li anode exhibits promising cycle stability when coupled with both Li-containing (LiNi 0.8 Co 0.15 Al 0.05 O 2 ) and Li-free (sulfur) cathodes.
Intrinsically sodiophilic, mesoporous metal-free wetting layers based on inexpensive carbon black for sodium-metal batteries
In this article, elevated temperature molten Na batteries are seeing a resurgence of interest for low-cost electrochemical energy storage for the grid. Of the many recent innovations in this battery concept, new methods focused on intermediate temperature operation (e.g. 110–190 °C) have gained prominence as a way to enable comparable performance with less thermal energy loss and lower-cost materials of construction. However, the poor wettability of molten Na on suitable solid-electrolyte separators such as sodium Beta Alumina Solid-Electrolyte (Na-β”-Al 2 O 3 , ‘BASE’) requires continued innovation in interface engineering to promote full utilization of the solid-electrolyte surface area and minimize cell resistance. There have been many successful approaches to improve Na-wettability to-date including heat treatment in an inert atmosphere to remove adsorbed surface species, deposition of alloying metals such as Pb, Sn, or Bi, and use of carbon-based interfacial layers. However, these approaches either lack the ability to provide good wetting at very low temperatures (near the melting point of Na) or rely on non-scalable processes and/or toxic/expensive metals. To solve these issues, a new carbon-based sodiophilic treatment is demonstrated, which utilizes inexpensive components to form a meso/macroporous sodiophilic layer, is easily applied via drop-casting or spray-coating, provides excellent wetting as low as 110 °C, and is completely metal-free. It is found that the good sodium wetting can be attributed to the wider range of pore sizes in the carbon layers demonstrated in this study. Na wetting may occur as surface tension is initially broken by larger pores, followed by the intrusion of molten Na into smaller pores due to the apparent intrinsic affinity of Na-metal for carbon surfaces, in conjunction with the capillarity effect. Low cell-level area specific resistances of 20–30 and 13–15 Ω·cm 2 are demonstrated at 110 and 140 °C respectively. Finally, the utility of this metal-free wetting layer for solid-Na anodes is explored, showing that the metal-free wetting layer can reach a critical current density of 1.88 mA·cm -2 at 30 °C.
Sequentially coupled flow and geomechanical simulation with a discrete fracture model for analyzing fracturing fluid recovery and distribution in fractured ultra-low permeability gas reservoirs
More accurate characterization and prediction of the in-situ distribution of fracturing fluid in fractured reservoirs are needed for enhancing well productivity. In this study, an implicit-sequentially coupled flow/geomechanics simulator incorporating an efficient discrete fracture model is developed to model fluid distribution and recovery performance of ultra-low permeability gas reservoirs. The finite-volume and finite-element methods are used for space discretization of the flow and geomechanics equations, respectively, while the backward Euler method is employed for time discretization. The flow and geomechanics equations are solved sequentially based on fixed-stress splitting. An efficient discrete-fracture model is used to explicitly model the fractured system. Flexible unstructured gridding is employed to model arbitrarily-oriented fractures. The interrelations among pore volume, permeability and geomechanical conditions are considered dynamically using two-way coupled flow and geomechanics computations. The geometry of fracture (networks) due to hydraulic fracturing has significant impacts on the fracturing fluid recovery efficiency and ensuing fluid distribution. Under the same injection volume, the fracturing fluid recovery is higher when the fracture geometry is planar. Fluid recovery is relatively lower whenever natural fractures are activated during fracturing treatments; flowback time is also shortened when complex fracture network with enlarged fracture interface is present. Fracturing fluid in hydraulic fractures may leak off into the natural fractures and subsequently imbibes into the surrounding matrix due to capillarity effects. The fracturing fluid recovery and in-situ fluid distribution are sensitive to the shut-in duration and fracture closure behavior. This study analyzes the coupled flow-geomechanical responses of fractured gas reservoirs during the post-fracturing periods. Understanding the fate of the fracturing fluid can provide insights on, to some extent, the stimulated fracture volume, size of the water invasion zone, and efficiency of the fracturing design. The simulation predictions can also provide more accurate initial reservoir conditions (e.g. distributions of different phases and pressure) for long-term well performance estimation.
Rain waves-wind waves interaction application to scatterometry
Modulation of a rain wave pattern by longer waves has been studied. An analytical model taking into account capillarity effects and obliquity of short waves has been developed. Modulation rates in wave number and amplitude have been computed. Experiments were carried out in a wave tank. First results agree with theoretical models, but higher values of modulation rates are measured. These results could be taken into account for understanding the radar response from the sea surface during rain.
A Novel Relative Permeability Model for Gas and Water Flow in Hydrate-Bearing Sediments With Laboratory and Field-Scale Application
In a producing gas hydrate reservoir the effective porosity available for fluid flow constantly changes with dissociation of gas hydrate. Therefore, accurate prediction of relative permeability using legacy models (e.g. Brooks-Corey (B-C), van Genuchten, etc.) that were developed for conventional oil and gas reservoirs would require empirical parameters to be calibrated at various S h over its range of variation, but such calibrations are precluded because of lack of experimental relative permeability data. This study proposes a new relative permeability model for gas hydrate-bearing media that is a function of maximum capillary pressure, capillary entry pressure, pore size distribution index, residual saturations, hydrate saturation, and four other constants. The three novel features of the proposed model are: (i) requires fitting its six empirical parameters only once using experimental data from any single S h , and the same set of empirical parameters predict relative permeability at all S h , (ii) includes the effect of capillarity, and (iii) includes the effect of pore-size distribution. From practical standpoint, the model can be used to simulate multiphase flow in gas hydrate-bearing sediments where the proposed relative permeability can account for the evolving hydrate saturation. The proposed model is implemented in a numerical simulator and the wall time required to perform simulations using the proposed model is shown to be similar to the time it takes to run same simulations with the B-C model. The proposed model is a step forward towards achieving the goal of physically accurate modeling of multiphase flow for gas hydrate-bearing sediments that accounts for the effect of gas hydrate saturation change on relative permeability.
Temperature effects on adsorption and capillarity water retention mechanisms in constrained unsaturated soils
Abstract This paper focuses on the impact of elevated temperatures on the adsorptive and capillarity water retention mechanisms of unsaturated soils under constrained (constant volume) conditions. This topic is critical for simulating the thermo-hydraulic behavior of soils in hydrogeological or geotechnical applications, including climate change effects on near surface soils, energy piles or soil borehole thermal energy storage systems in unsaturated soil layers, and buffers for geological nuclear waste repositories. A nonisothermal soil water retention curve (SWRC) that separately considers the temperature-dependency of the key parameters governing adsorptive and capillarity water retention mechanisms and soil physical parameters (e.g., surface tension, contact angle, adsorption capacity, cation exchange capacity, mean cavitation suction, air entry value and equilibrium film thickness) was developed to provide insights into the impact of temperature on water retention over the full suction range. The nonisothermal SWRC was validated using experimental data on high plasticity clays, with a good prediction of temperature effects on adsorption and capillarity water retention mechanisms in constrained unsaturated soils.
A generalized 3D elastic model for nanoscale, self-assembled oxide-metal thin films with pillar-in-matrix configurations
In recent years, functional oxide-metal based vertically aligned nanocomposite (VAN) thin films have gained interest due to their intriguing physical properties and multifunctionalities stemming from the complex interactions between the two phases in the film and the substrate. In this work, we develop a model for studying the energetics of these thin film systems, including the effects of both lattice mismatch and capillary forces due to interface curvature. Each phase is incorporated into the model using a phase indicator function, and we introduce the capillary forces as body forces using a vector density representation of the interface. The model is implemented using the finite element method to study the deformation of the thin film which is composed of Au nanopillars embedded in a La 0.7 Sr 0.3 MnO 3 (LSMO) matrix on an SrTiO 3 (STO) substrate. Further, the results suggest that the total energy is lowest for random configurations of pillars compared to ordered square and hexagonal lattice configurations, consistent with the random distribution of pillars found in experiments. Furthermore, we find that the interfacial energy dominates the total energy of each configuration, suggesting that interfacial energy in the system is an important design parameter for nanocomposite growth, along with the lattice mismatch.
Controlling matric potential in microfluidics to examine microbial dynamics in unsaturated porous media
The use of microfluidics for the study of soil microbial ecology is an emerging field. Most microfluidic studies of biological systems, however, have been performed under fully saturated conditions that are not representative of natural soil. Therefore, while microfluidics offer many unique capabilities that other methodologies cannot, they are not currently suited to address the effects of matric potential, an important variable defining the microbial moisture niche. Here, a methodology is presented that allows the user to control the aqueous conditions within microfluidic networks by manipulating matric potential using a hanging water column. The method relies on hydrophilic surface treatment of the microfluidic device using polyvinyl alcohol (PVA) and incorporating a bed of small pores at the network boundaries, which serve as a porous ceramic plate analogue (PPA). The method was validated on a simple capillary bundle and then on a more complex pore network. A water retention curve, exhibiting hysteresis, was generated for the pore network over a narrow matric potential range of 0 to – 5 kPa. Both the drainage and wetting curves were reproducible, as were the spatial configuration and the number of fragmented moisture niches in the pore network, particularly on the drainage curve. In contrast, the wetting curve exhibited greater variability in spatial configuration due to the “ink bottle effect,” where capillarity was interrupted by wider pore bodies. Ultimately, the methodology provides realistic pore-scale moisture conditions that can be easily manipulated and maintained, enabling new opportunities to explore soil biophysics and microbial biogeography in unsaturated porous media. As a brief example, images showing the localization of fluorescently tagged Pantoea sp. YR343 at −4.3 kPa are presented, highlighting bacterial distributions in water films and air-water interfaces.
Two phase flow and heat transfer in porous beds under variable body forces, part 2
Analytical and experimental investigations of a pilot model of a channel for the study of two-phase flow under low or zero gravity are presented. The formulation of dimensionless parameters to indicate the relative magnitude of the effects of capillarity, gravity, pressure gradient, viscosity, and inertia is described. The investigation is based on the principal equations of fluid mechanics and thermodynamics. Techniques were investigated by using a laser velocimeter for measuring point velocities of the fluid within the porous material without disturbing the flow.
Electrohydrodynamic heat pipes.
An electrohydrodynamic heat pipe of radical design is proposed which substitutes polarization electrohydrodynamic force effects for capillarity in collecting, guiding, and pumping a condensate liquid phase. The discussed device is restricted to the use of dielectric liquids as working fluids. Because of the relatively poor thermal transport properties of these liquids, capillary heat pipes using these liquids have not been high performance devices. The employment of the electrohydrodynamic concept should enhance this performance and help fill the performance gap that exists in the temperature range from 250 F to 750 F for 'conventional' capillary heat pipes.
The Effect of Solidification Rate on Morphological Stability
At low solidification rates, the criterion for the onset of morphological instability parallels closely the criterion of constitutional supercooling. At somewhat larger rates of solidification, however, the results of the perturbation theory of morphological instability differ significantly from the predictions of constitutional supercooling. This arises because the critical wave length for instability decreases as solidification rate increases and thus the effects of capillarity (solid-liquid surface tension) play a strong stabilizing role. This gives rise to the concept of absolute stability, according to which the system will always be stable for a sufficiently large rate of solidification. This enhanced stabilization by capillarity is present only so long as local equilibrium is maintained at the solid-liquid interface. If the interfacial temperature drops below its equilibrium value by an amount dependent on growth rate, oscillatory morphological instabilities can occur. The differences among these various stability criteria are illustrated by means of some simple two-dimensional diagrams that should supplant the conventional plots of (temperature gradient)/(growth rate) vs. alloy concentration.
Liquid-Vapor Interface Configurations Investigated in Low Gravity
The Interface Configuration Experiment (ICE) is part of a multifaceted study that is exploring the often striking behavior of liquid-vapor interfaces in low-gravity environments. Although the experiment was posed largely as a test of current mathematical theory, applications of the results should be manifold. In space almost every fluid system is affected, if not dominated, by capillarity (the effects of surface tension). As a result, knowledge of fluid interface behavior, in particular an equilibrium interface shape from which any analysis must begin, is fundamental--from the control of liquid fuels and oxygen in storage tanks to the design and development of inspace thermal systems, such as heat pipes and capillary pumped loops. ICE has increased, and should continue to increase, such knowledge as it probes the specific peculiarities of current theory upon which our present understanding rests. Several versions of ICE have been conducted in the drop towers at the NASA Lewis Research Center, on the space shuttles during the first and second United States Microgravity Laboratory missions (USML-1 and USML-2), and most recently aboard the Russian Mir space station. These studies focused on interfacial problems concerning the existence, uniqueness, configuration, stability, and flow characteristics of liquid-vapor interfaces. Results to date have clearly demonstrated the value of the present theory and the extent to which it can predict the behavior of capillary systems.
Hydrodynamics of Two-Phase Flows through Porous Media in Microgravity: Packed Bed Reactor Experiment onboard of the International Space Station
The objective of the Packed Bed Reactor Experiment was to develop a fundamental understanding of the hydrodynamics of two-phase flow with no phase transition through porous media in microgravity. This work describes two experimental campaigns flown on the International Space Station (ISS) that were designed to achieve the objective. This work presents the results on flow patterns observed, two-phase flow pressure drop in porous media, and the impact of capillary effects on pressure drop at various gas and liquid flow rates. This work is the first to present predictive correlations of the two-phase friction factor for the different regimes identified based on the superficial liquid and gas velocity in microgravity, the first to hypothesize the different regimes based on the change in slope of the pressure gradient versus flow rate plots, the first to address the effects of the capillarity on the pressure gradient and the first to measure column holdup and assess the effective porosity based on the packing and the trapped gas bubbles. Experimental data on pressure drop in gas (N2) – liquid (water) flow show the presence of four different flow regimes in microgravity. Dispersed bubble flow (DB) and pulse (P) flow regimes are detected at high liquid flow rates, whereas at low liquid flow rates “large bubble” or elongated bubble (LB) and “gas channeling” (GC) regimes are observed. For these different flow regimes, different two-phase flow friction factor and pressure gradient correlations are presented for the first time as a function of the gas and liquid modified Reynolds numbers and Suratman number. Within the viscous-capillary (V-C) regime, it is found that the capillary contribution is the dominant force that contributes to the pressure drop for the wetting case (glass). However, for the non-wetting packing (Teflon), the viscous contribution dominates. It was found that the gas hold-up and pressure drop are functions of bed history at low liquid and gas flow rates with the magnitude of the hysteresis decreasing with increasing flow rates. PBRE-2 results show that the capillary force is a strong function of the superficial liquid velocity but is a much weaker function of the superficial gas velocity and varies inversely with the particle diameter. Within the Viscous-Capillary (V-C) regime, over 90% of the pressure gradient is attributed to the capillary contribution in the gas continuous regime. However, in the large bubble regime, the viscous and capillary contributions were comparable. After the completion of PBRE-2 with glass spherical beads, another bed packed with alumina was installed. Pressure gradient data for the alumina packed bed (PBRE-Water Recovery) were transferred to the PI and were not analyzed by the authors of this work. The Packed Bed Reactor Experiment concluded its on-orbit operation after two successful campaigns of testing in 2017 and in 2021. The flight hardware was brought back from orbit and is being reconditioned for a series of future experiments referred to as PBRE-WRS in support of water recovery (WRS). The WRS series consists of testing different two-phase fluid system components and packed beds to assess their pressure gradient characteristics, which will be used for designing packed bed reactors for various applications relevant to life support. Although there is so much relevance of the experimental results obtained from the two PBRE campaign in microgravity to life support, these findings also apply to other applications that involve two phase flow in porous medium such as fuel cells, transport of nutrient to plants in space and other chemical and materials processing that involve two phase flows. These systems operate differently in microgravity because, due to the lack of buoyancy, the density difference between the phases becomes irrelevant and no longer leads to phase separation.
Initial conditions implied by t exp 1/2 solidification of a sphere with capillarity and interfacial kinetics
The paper explores the initial conditions implied by t exp 1/2 growth of a spherical crystal solidifying from a pure, undercooled melt, including the effects of both capillarity and interface kinetics, and relates the findings to initial conditions that would be expected on the basis of classical nucleation theory. For crystal sizes near the nucleation radius, the calculated temperature profiles show a cold region ahead of the advancing interface that is even more undercooled than the undercooled bath. This cold region acts as a local heat sink that compensates for the reduced growth speed that would otherwise result from capillarity and kinetics, leading to precisely the same t exp 1/2 growth law that would have been obtained had both capillarity and kinetics been neglected.
Exploring in aerospace rocketry. 8 - Zero gravity effects
Weightlessness in space, capillarity and surface energy, and behavior of liquids in zero gravity