Oliver Trötschler

Abstract

Abstract Density-driven dissolution of carbon dioxide in water is a well-known and much described mechanism in geological sequestration of this greenhouse gas. It is remarkable that such enhanced dissolution does not receive attention in karst hydrology and speleology. Models and hypotheses on karst development are complex and consider many different processes. We focus here on the influence of CO2 partial gas pressures at the interface between atmosphere and karst water on the dynamics of dissolved CO2 concentrations below the water table. Seasonal variations of microbial soil activity and root respiration or barometric-pressure changes cause fluctuations in CO2 partial pressures. Dependent on the existence and strength of a karst-water background flow, fingering regimes might be triggered causing enhanced dissolution of CO2. This allows replenishment of CO2, and, thus, dissolutional power even deep in the water body without the need for percolating water to transport dissolved CO2. We present and discuss simplified and generic experimental and computational scenarios to strengthen our claim, and we try to give answers to: how much? and under which circumstances? The applied numerical model solves the Navier-Stokes equation with water density dependent on CO2 concentration and temperature. We show that calculated CO2 mass fluxes into the water bodies are dependent on the ratio of Péclet to Rayleigh numbers (Pe/Ra) and show a local minimum around Pe/Ra = 1, i.e. when natural and forced convection are about equal. Concluding, we claim that there is sufficient reason to consider density-driven dissolution as a process of relevance in karstification if circumstances are given.

Abstract

Carbon dioxide density-driven dissolution in a water-filled laboratory flume of the dimensions 60 cm length, 40 cm height, 1 cm thickness, was visualized using a pH-sensitive color indicator. We focus on atmospheric pressure conditions, like in caves where CO2 concentrations are typically higher. Varying concentrations of carbon dioxide were applied as boundary conditions at the top of the experimental setup, leading to the onset of convective fingering at differing times. The data were used to validate a numerical model implemented in the numerical simulator DuMux. The model solves the Navier–Stokes equations for density-induced water flow with concentration-dependent fluid density and a transport equation, including advective and diffusive processes for the carbon dioxide dissolved in water. The model was run in 2D, 3D, and pseudo-3D on two different grids. Without any calibration or fitting of parameters, the results of the comparison between experiment and simulation show satisfactory agreement with respect to the onset time of convective fingering, and the number and the dynamics of the fingers. Grid refinement matters, in particular, in the uppermost part where fingers develop. The 2D simulations consistently overestimated the fingering dynamics. This successful validation of the model is the prerequisite for employing it in situations with background flow and for a future study of karstification mechanisms related to CO2-induced fingering in caves.