For longer than one decade, liquid metal batteries (LMBs) are developed with the primary aim to provide economic stationary energy storage. Featuring two liquid metal electrodes separated by a molten salt electrolyte, LMBs operate at elevated temperature as simple concentration cells. Therefore, efficient mass transfer is a basic prerequisite for their economic operation. Understanding these mechanisms cannot be limited at the single layer level. With this motivation, the effects of solutal- and thermally-driven flow are studied, as well as the flow coupling between the three liquid layers of the cell. It is shown that solutal convection appears first and thermal convection much later. While the presence of solutal flow depends on the mode of operation (charge or discharge), the occurrence of thermal convection is dictated by the geometry (thickness of layers). The coupling of the flow phenomena between the layers is intriguing: while thermal convection is confined to its area of origin, i.e. the electrolyte, solutal convection is able to drive flow in the positive electrode and in the electrolyte.
We numerically examine solutal convection in porous media, driven by the dissolution of carbon dioxide (CO2) into water---an effective mechanism for CO2 storage in saline aquifers. Dissolution is associated with slow diffusion of free-phase CO2 into the underlying aqueous phase followed by density-driven convective mixing of CO2 throughout the water-saturated layer. We study the fluid dynamics of CO2 convection in the single aqueous-phase region. A comparison is made between two different boundary conditions in the top of the formation: (i) a constant, maximum aqueous-phase concentration of CO…
We study the fractionation of two components between a well-mixed gas and a saturated convecting porous layer. Motivated by geological carbon dioxide (CO$_2$) storage we assume that convection is driven only by the dissolved concentration of the first component, while the second acts as a tracer with increased diffusivity. Direct numerical simulations for convection at high Rayleigh numbers reveal that the partitioning of the components, in general, does not follow a Rayleigh fractionation trend, as commonly assumed. Initially, increases in tracer diffusivity also increase its flux, because th…
Interfacial tension gradients drive flow along liquid-liquid interfaces in a process known as the Marangoni effect. Such gradients can be caused by surfactants, which has been extensively studied in the literature. Less is known of its nanoscale properties, where molecular interfaces display properties separate from bulk liquid matter such as interfacial viscosity. In this report we study the molecular solutal Marangoni effect using molecular dynamics simulations. We show that molecular interfacial effects are important and should be accounted for in nanofluidic regimes. Hydrodynamic models ca…
We describe an interpretation of convection in binary fluid mixtures as a superposition of thermal and solutal problems, with coupling due to advection and proportional to the separation parameter S. Many properties of binary fluid convection are then consequences of generic properties of 2 x 2 matrices. The eigenvalues of 2 x 2 matrices varying continuously with a parameter r undergo either avoided crossing or complex coalescence, depending on the sign of the coupling (product of off-diagonal terms). We first consider the matrix governing the stability of the conductive state. When the therma…
We theoretically investigate the role of solutal free convection on the diffusion of a buoyant solute at the microfluidic scales, $\simeq 5$--$500~μ$m. We first consider a horizontal microfluidic slit, one half of which initially filled with a binary solution (solute and solvent), and the other half with pure solvent. The buoyant forces generate a gravity current that couples to the diffusion of the solute. We perform numerical resolutions of the 2D model describing the transport of the solute in the slit. This study allows us to highlight different regimes as a function of a single parameter,…
Liquid Metal Batteries (LMBs) are a promising grid-scale energy storage technology that offer low costs per kilowatt-hour, high energy and current densities, as well as low fade rates. The all-liquid composition of the batteries, as well as the presence of temperature gradients and electric and magnetic fields, result in the occurrence of multiple fluid phenomena. These can affect the hydrodynamic stability of the battery, thereby making their interactions critical to understand. In this work, the interaction of Rayleigh-Bénard convection and Electro-vortex flow is investigated as these types …
Evaporating salty droplets are ubiquitous in nature, in our home and in the laboratory. Interestingly, the transport processes in such apparently simple systems differ strongly from evaporating "freshwater" droplets since convection is partly inverted due to Marangoni stresses. Such an effect has crucial consequences to the salt crystallization process and to the deposits left behind. In this work we show unprecedented measurements that, not only confirm clearly the patterns of the flow inversion, but also elucidate their impact on the distribution of non-volatile solutes. Contrary to what has…
Liquid Metal Batteries (LMBs) are a promising concept for cheap electrical energy storage at grid level. These are built as a stable density stratification of three liquid layers, with two liquid metals separated by a molten salt. In order to ensure a safe and efficient operation, the understanding of transport phenomena in LMBs is essential. With this motivation we study thermal convection induced by internal heat generation. We consider the electrochemical nature of the cell in order to define the heat balance and the operating parameters. Moreover we develop a simple 1D heat conduction mode…
Convective motions in a fluid layer are affected by its orientation with respect to the gravitational field. We investigate the long-term stability of a thermally-stressed layer of a binary liquid mixture and show that pattern formation is strongly affected by marginal inclinations as small as a few milliradians. At small Rayleigh numbers the mass transfer is dominated by the induced large scale shear flow, while at larger Rayleigh numbers it is dominated by solutal convection. At the transition, the balance between the solutal and shear flows gives rise to drifting columnar flows moving in op…
Motivated by studies of the cylinder wake, in which the vortex-shedding frequency can be obtained from the mean flow, we study thermosolutal convection driven by opposing thermal and solutal gradients. In the archetypal two-dimensional geometry with horizontally periodic and vertical no-slip boundary conditions, branches of traveling waves and standing waves are created simultaneously by a Hopf bifurcation. Consistent with similar analyses performed on the cylinder wake, we find that the traveling waves of thermosolutal convection have the RZIF property, meaning that linearization about the me…
In this paper, the instability of layered two-phase flows caused by the presence of a soluble surfactant (or a surface active solute) is studied. The fluids have different viscosities, but are density matched to focus on Marangoni effects. The fluids flow between two flat plates, which are maintained at different solute concentrations. This establishes a constant flux of solute from one fluid to the other in the base state. A linear stability analysis is performed, using a combination of asymptotic and numerical methods. In the creeping flow regime, Marangoni stresses destabilize the flow, pro…
Thermal convection in a horizontal layer with uniform internal heating and stress-free constant-temperature boundaries is analyzed numerically. The work is motivated by the questions arising in development of liquid metal batteries, in which convection is induced by the Joule heating of electrolyte. It is demonstrated that three-dimensional convection cells exist at subcritical Rayleigh numbers.
Liquid metal batteries (LMBs) were recently proposed as cheap large scale energy storage. Such devices are urgently required for balancing highly fluctuating renewable energy sources. During discharge, intermetallic phases tend to form in the cathode of LMBs. These do not only limit the up-scalability, but also the efficiency of the cells. Generating a mild fluid flow in the fully liquid cell will smoothen concentration gradients and minimise the formation of intermetallics. In this context we study electro-vortex flow numerically. We simulate a recent LMB related experiment and discuss how th…
Liquid metal batteries are proposed for low-cost grid scale energy storage. During their operation, solid intermetallic phases often form in the cathode and are known to limit the capacity of the cell. Fluid flow in the liquid electrodes can enhance mass transfer and reduce the formation of localized intermetallics, and fluid flow can be promoted by careful choice of the locations and topology of a battery's electrical connections. In this context we study four phenomena that drive flow: Rayleigh-Bénard convection, internally heated convection, electro-vortex flow, and swirl flow, in both expe…
Oscillatory droplet dissolution from competing Marangoni and gravitational flows
University of Twente（特温特大学）；Department of Chemical and Materials Engineering, University of Alberta（阿尔伯塔大学化学与材料工程系）；Max Planck Institute for Dynamics and Self-Organization（马克斯·普朗克动力学与自组织研究所）
The design and performance of liquid metal batteries, a new technology for grid-scale energy storage, depend on fluid mechanics because the battery electrodes and electrolytes are entirely liquid. Here we review prior and current research on the fluid mechanics of liquid metal batteries, pointing out opportunities for future studies. Because the technology in its present form is just a few years old, only a small number of publications have so far considered liquid metal batteries specifically. We hope to encourage collaboration and conversation by referencing as many of those publications as …
Generation of thermal convection flow in the liquid metal battery, a device recently proposed as a promising solution for the problem of the short-term energy storage, is analyzed using a numerical model. It is found that convection caused by Joule heating of electrolyte during charging or discharging is virtually unavoidable. It exists in laboratory prototypes larger than a few cm in size and should become much stronger in larger-scale batteries. The phenomenon needs further investigation in view of its positive (enhanced mixing of reactants) and negative (loss of efficiency and possible disr…
We present a novel laboratory setup for studying the fluid dynamics in liquid metal batteries (LMBs). LMBs are a promising technology suited for grid-scale energy storage, but flows remain a confounding factor in determining their viability. Two important drivers of flow are thermal gradients, caused by internal heating during operation, and electrovortex flow (EVF), induced by diverging current densities. Our setup explores thermal gradients and electrovortex flow separately and in combination in a cylindrical layer of liquid gallium, simulating the behavior in a single layer of an LMB. In th…
Fluid dynamics of mixing in the tanks of small vanadium redox flow batteries: Insights from order-of-magnitude estimates and transient two-dimensional simulations
The present study aims to investigate the study of double-diffusive convection on peristaltic flow under the assumption of long wavelength and low Reynolds number. The mathematical modelling for a two dimensional flow, along with double diffusion in nanofluids is considered. The motivation of the present research work is to analyse the effects of thermal radiation on a peristaltic flow through a porous medium in a non-uniform channel.The heat flux of the linear approximation employs the thermal radiation ofthe flow problem. The governing equations are analytically solved by using Homotopy Pert…
Active oil droplets in a liquid are believed to repel due to the Marangoni effect, while buoyancy effects caused by the density difference between the droplets, diffusing product, and ambient fluid are usually overlooked. Recent experiments have observed active droplet clustering phenomena due to buoyancy-driven convection (Kruger et al. Eur. Phys. J. E, vol. 39, 2016, pp.1-9). In this study, we numerically analyze the buoyancy effect in addition to Marangoni flow, characterized by Peclet number $Pe$. The buoyancy effects originate from (i) the density difference between the droplet and the am…
