Density-driven convection enhances the carbon dissolution rate, which is significant for the geological carbon storage. This process will also influence the spatiotemporal pH and carbon concentrations of the underground fluid. To illuminate the convection mechanism, it is critical to understand the evolution of those properties within the porous media. However, determining the spatiotemporal pH and concentration within porous media is always challenging. This study employed a combination of three pH indicators that can track a wide range in pH from 4 to 9.5 in a convection experiment. Furthermore, we compared three image-processing techniques: Hue, gray-difference, and angular representation of RGB color space $\mathbf{(ϕ,θ)}$ for quantifying color changes from the universal $\text{pH}$ indicator arising from the carbon convection. The characterized colors were mapped into pH by calibrating against benchmark solutions. The comparative results demonstrate that the color quantified by the Hue technique is most robust, showing invariance to fluid thickness, camera settings, and LED luminance. In the convection experiments, it produces a continuous spatial distribution of pH and concentration level in the system. In contrast, the $\mathbf{(ϕ,θ)}$ and gray-difference techniques were more sensitive to environmental variations. They also have significant limitations for $\text{pH}$ interpolation in the critical range due to their non-monotonic calibration paths. Although all methods ultimately produced similar estimates of total dissolved carbon, the Hue technique offers greater stability and universality for high-resolution, dynamic measurements of pH and carbon concentration in the convection experiments.
While there has been a large interest in studying the role of dissolution-driven free convection in the context of geological sequestration, the contribution of forced convection has been largely ignored. This manuscript considers CO$_2$ sequestration in saline aquifers with natural background flow and uses theoretical arguments to compute the critical background velocity needed to establish the forced convective regime. The theoretical arguments are supported by two dimensional high-resolution numerical simulations which demonstrate the importance of forced convection in enhancing dissolution…
Enhancing the efficiency of water electrolysis, which can be severely impacted by the nucleation and growth of bubbles, is key in the energy transition. In this combined experimental and numerical study, in-situ bubble evolution and dissolution processes are imaged and compared to numerical simulations employing the immersed boundary method. We find that it is crucial to include solutal driven natural convection in order to represent the experimentally observed bubble behaviour even though such effects have commonly been neglected in modelling efforts so far. We reveal how the convective patte…
Motivated by geological carbon dioxide (CO$_2$) storage, many recent studies have investigated the fluid dynamics of solutal convection in porous media. Here we study the convective dissolution of CO$_2$ in a closed system, where the pressure in the gas declines as convection proceeds. This introduces a negative feedback that reduces the convective dissolution rate even before the brine becomes saturated. We analyse the case of an ideal gas with a solubility given by Henry's law, in the limits of very low and very high Rayleigh numbers. The equilibrium state in this system is determined by the…
We present the first experiments of dissolution-driven convection of carbon dioxide (CO$_2$) in a confined brine-saturated porous medium at high pressures. We designed a novel Hele-Shaw cell that allows for both visual and quantitative analyses, and address the effects of free-phase CO$_2$ and brine composition on convective dissolution. The visual examination of the gas volume combined with the measurement of pressure, which both evolve with dissolution, enable us to yield insights into the dynamics of convection in conditions that more closely reflect the geologic conditions. We find and ana…
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…
Chemical reactions can accelerate, slow down or even be at the very origin of the development of dissolution-driven convection in partially miscible stratifications, when they impact the density profile in the host fluid phase. We numerically analyze the dynamics of this reactive convective dissolution in the fully developed non-linear regime for a phase A dissolving into a host layer containing a dissolved reactant B. We show that for a general A+B$\rightarrow$C reaction in solution, the dynamics vary with the Rayleigh numbers of the chemical species, i.e. with the nature of the chemicals in …
We numerically investigate both single and multiple droplet dissolution with droplets consisting of lighter liquid dissolving in a denser host liquid. The significance of buoyancy is quantified by the Rayleigh number Ra which is the buoyancy force over the viscous damping force. In this study, Ra spans almost four decades from 0.1 to 400. We focus on how the mass flux, characterized by the Sherwood number Sh, and the flow morphologies depend on Ra. For single droplet dissolution, we first show the transition of the Sh(Ra) scaling from a constant value to $Sh\sim Ra^{1/4}$, which confirms the e…
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 lifetime $τ$ of an isothermal and purely diffusively dissolving droplet in a host liquid scales as $τ\sim R_0^2$ with its initial radius $R_0$ [Langmuir, Phys. Rev. 12, 368 (1919)]. For a droplet dissolving due to natural convection driven by density differences, its lifetime scales as $τ\sim R_0^{5/4}$ [Dietrich et al., J. Fluid Mech. 794, 45 (2016)]. In this paper we experimentally find and theoretically derive yet another droplet dissolution behavior, resulting in $τ\sim R_0^4$. It occurs when the dissolution dynamics is controlled by local heating of the liquid, leading to a modified s…
The dissolution of solids has created spectacular geomorphologies ranging from centimeter-scale cave scallops to the kilometer-scale "stone forests" of China and Madagascar. Mathematically, dissolution processes are modeled by a Stefan problem, which describes how the motion of a phase-separating interface depends on local concentration gradients, coupled to a fluid flow. Simulating these problems is challenging, requiring the evolution of a free interface whose motion depends on the normal derivatives of an external field in an ever-changing domain. Moreover, density differences created in th…
We explore the chaotic dynamics of Rayleigh-Bénard convection using large-scale, parallel numerical simulations for experimentally accessible conditions. We quantify the connections between the spatiotemporal dynamics of the leading-order Lyapunov vector and different measures of the flow field pattern's topology and dynamics. We use a range of pattern diagnostics to describe the spatiotemporal features of the flow field structures which includes many of the traditional diagnostics used to describe convection as well as some diagnostics tailored to capture the dynamics of the patterns. Using p…
Geological storage of CO$_2$ in deep saline aquifers is a promising measure to mitigate global warming by reducing the concentration of this greenhouse gas in the atmosphere. When CO$_2$ is injected in the geological formation, it dissolves partially in the interstitial brine, thus rendering it denser than the CO$_2$-devoid brine below, which creates a convective instability. The resulting convection accelerates the rate of CO$_2$ perennial trapping by dissolution in the brine. The instability and resulting convection have been intensively discussed by numerical and theoretical approaches at t…
The density-driven convection coupled with chemical reaction is the preferred mechanism for permanently storing CO2 in saline aquifers. This study uses a 2D visual Hele-Shaw cell to evaluate and visualize the density-driven convection formed due to gravitational instabilities, also known as Rayleigh-Taylor instability. The primary goal of the experiments is to understand the various mechanisms for the mass transfer of gaseous CO2 into brine with different initial ionic concentrations and flow permeability. Moreover, the impact of CO2 flow rates, injection locations, reservoir dipping angle, an…
In many environmental and industrial applications, the mass transfer of gases in liquid solvents is a fundamental process during the generation of bubbles for specific purposes or, vice versa, the removal of entrapped bubbles. We address the growth dynamics of a trapped slug bubble in a vertical glass cylinder under a water barrier. In the studied process, the ambient air atmosphere is replaced by a CO$_2$ atmosphere at the same or higher pressure. The asymmetric exchange of the gaseous solutes between the CO$_2$-rich water barrier and the air-rich bubble always results in net bubble growth. W…
We present a phenomenological theory for spatiotemporal chaos (STC) in Rayleigh-Benard convection, based on the generalized Swift-Hohenberg model. We apply a random phase approximation to STC and conjecture a scaling form for the structure factor $S(k)$ with respect to the correlation length $ξ_2$. We hence obtain analytical results for the time-averaged convective current $J$ and the time-averaged vorticity current $Ω$. We also define power-law behaviors such as $J \sim ε^μ$, $Ω\sim ε^λ$ and $ξ_2 \sim ε^{-ν}$, where $ε$ is the control parameter. We find from our theory that $μ= 1$, $ν\ge 1/2$…
Pools of carbon dioxide are found in natural geological accumulations and in engineered storage in saline aquifers. It has been thought that once this CO2 dissolves in the formation water, making it denser, convection streams will transport it efficiently to depth, but this may not be so. Here, we assess theoretically and experimentally the impact of natural chemical reactions between the dissolved CO2 and the rock formation on the convection streams in the subsurface. We show that, while in carbonate rocks the streaming of dissolved carbon dioxide persists, the chemical interactions in silica…
