Convective carbon dioxide dissolution in a closed porous medium at high-pressure real-gas conditions

TL;DR

This study models and experimentally verifies the convective dissolution of CO2 in a closed porous medium under high-pressure real-gas conditions, highlighting the effects of pressure-dependent properties on dissolution dynamics.

Contribution

It extends previous low-pressure ideal-gas models to high-pressure real-gas conditions, incorporating compressibility and solubility effects, and validates the models with experiments and simulations.

Findings

Models accurately predict convective CO2 dissolution dynamics.

Pressure decay experiments determine dissolution flux prefactors.

Negative feedback from pressure drop weakens at higher pressures.

Abstract

We combine modeling and measurements to investigate the dynamics of convective carbon dioxide (CO$_2$) dissolution in a pressure-volume-temperature cell, extending a recent study by Wen et al. (J. Fluid Mech., vol. 854, 2018, pp. 56--87) at low-pressure under ideal-gas conditions to high-pressure and real-gas conditions. Pressure-dependent compressibility and solubility are included to model the evolution of CO$_2$ concentration in the gas phase and at the interface, respectively. Simple ordinary-differential-equation models are developed to capture the mean behavior of the convecting system at large Rayleigh number and are then verified by using both numerical simulations and laboratory experiments. The prefactor for the linear scaling of convective CO$_2$ dissolution is evaluated -- for the first time -- by using pressure-decay experiments in bead packs at reservoir conditions. The results show that our models could quantitatively predict the process of the convective CO$_2$ dissolution in pressure-decay experiments. Moreover, the results also reveal that for increasing gas pressure in closed systems, the negative feedback of the pressure drop -- resulting from the dissolution of CO$_2$ in the liquid -- is weakened due to the decrease of the solubility constant at real-gas conditions. Our analysis provides a new direction for determination and validation of the convective dissolution flux of CO$_2$ in porous media systems.