CO$_2$ convective dissolution in a 3-D granular porous medium: an experimental study

TL;DR

This experimental study investigates CO₂ convective dissolution in a 3-D porous medium, revealing discrepancies with theoretical predictions and highlighting the influence of pore structure on convection and CO₂ flux.

Contribution

First experimental characterization of convective dissolution onset in 3-D porous media, showing larger growth rates and multi-scale flow features compared to theory.

Findings

Growth rate remains constant with varying CO₂ partial pressure

Measured growth rates are 1 to 3 orders of magnitude larger than predictions

Flow exhibits broad Fourier spectrum indicating multi-scale convection

Abstract

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 the Darcy scale, but few experimental studies have characterized them quantitatively. By using both refractive index matching and planar laser induced fluorescence, we measure for the first time the onset characteristics of the convective dissolution instability in a 3-D porous medium located below a gas compartment. Our results highlight that the dimensional growth rate of the instability remains constant when the CO$_2$ partial pressure in the compartment is varied, in clear discrepancy with the theoretical predictions. Furthermore, within the CO$_2$ partial pressure range studied, the measured growth rate is 1 to 3 orders of magnitude larger than the predicted value. The Fourier spectrum of the front is very broad, highlighting the multi-scale nature of the flow. Depending on the measurement method and CO$_2$ partial pressure, the mean wavelength is 1 to 3 times smaller than the predicted value. Using a theoretical model developed recently by Tilton (J.~Fluid Mech., 2018), we demonstrate that our experimental results are consistent with a forcing of convection by porosity fluctuations. Finally, we discuss the possible effects of this forcing by the porous medium's pore structure on the CO$_2$ flux across the interface, measured in our experiments about one order of magnitude higher than expected.