Numerical modeling of self-limiting and self-enhancing caprock alteration induced by CO2 storage in a depleted gas reservoir

Abstract

This paper presents numerical simulations of reactive transport which may be induced in the caprock of an on-shore depleted gas reservoir by the geological sequestration of carbon dioxide. The objective is to verify that CO 2 geological disposal activities currently being planned for the study area are safe and do not induce any undesired environmental impact.In our model, fluid flow and mineral alteration are induced in the caprock by penetration of high CO 2 concentrations from the underlying reservoir, where it was assumed that large amounts of CO 2 have already been injected at depth. The main focus is on the potential effect of precipitation and dissolution processes on the sealing efficiency of caprock formations.Concerns that some leakage may occur in the investigated system arise because the seal is made up of potentially highly-reactive rocks, consisting of carbonate-rich shales (calcite+dolomite averaging up to more than 30% of solid volume fraction). Batch simulations and multi-dimensional 1D and 2D modeling have been used to investigate multicomponent geochemical processes. Numerical simulations account for fracture-matrix interactions, gas 2 phase participation in multiphase fluid flow and geochemical reactions, and kinetics of fluidrock interactions.The geochemical processes and parameters to which the occurrence of high CO 2 concentrations are most sensitive are investigated by conceptualizing different mass transport mechanisms (i.e. diffusion and mixed advection+diffusion). The most relevant mineralogical transformations occurring in the caprock are described, and the feedback of these geochemical processes on physical properties such as porosity is examined to evaluate how the sealing capacity of the caprock could evolve in time.The simulations demonstrate that the occurrence of some gas leakage from the reservoir may have a strong influence on the geochemical evolution of the caprock. In fact, when a free CO 2 -dominated phase migrates into the caprock through fractures, or through zones with high initial porosity possibly acting as preferential flow paths for reservoir fluids, low pH values are predicted, accompanied by significant calcite dissolution and porosity enhancement. In contrast, when fluid-rock interactions occur under fully liquid-saturated conditions and a diffusion-controlled regime, pH will be buffered at higher values, and some calcite precipitation is predicted which leads to further sealing of the storage reservoir.

Investigation of CO2 Plume Behavior for a Large-Scale Pilot Test of Geologic Carbon Storage in a Saline Formation

“…As CO 2 -laden brine sinks deeper into the formation, it can set up circulation patterns that enable more free-phase CO 2 to come into contact with native brine, enabling more dissolution to occur (Ennis-King and Paterson 2005;Pruess and Zhang 2008). (4) Mineral trapping: CO 2 reacts with rock minerals to form carbonate compounds, typically over very long time scales Xu et al 2003Xu et al , 2005Gherardi et al 2007). The first three mechanisms, collectively referred to as hydrodynamic trapping by Bachu et al (1994), dominate plume behavior over the hundred-year time scale and are the focus of the present paper.…”

Molecular dynamics simulations of the electrical double layer on smectite surfaces contacting concentrated mixed electrolyte (NaCl–CaCl2) solutions

“…Following Tournassat et al [52], we focus on smectites because these ubiquitous clay mineral nanoparticles play important roles in soil chemistry [55,56], soil mechanics [57], fault friction [58,59], materials chemistry [60], landfill and contaminated site isolation [61,62], high-level radioactive waste storage [63,64], CO 2 sequestration [65,66], and gas hydrate stability in marine sediments [67,68]. Their adsorption properties for small inorganic ions have been extensively studied using macroscopic [55,56,69], spectroscopic [24,25], and MD simulation techniques [18,35,37,45,49,52].…”

Connecting the Molecular Scale to the Continuum Scale for Diffusion Processes in Smectite-Rich Porous Media

“…In the present paper, we address this abiding question for the particular case of the "apparent" diffusion coefficient D a [defined by the continuum-scale relation N i ≡ D a,i ∂C * /∂x i , if N i is the mass flux density of the species of interest along the x i direction and C * is its total concentration per volume of porous medium] of water tracers and dissolved solutes in smectiterich porous media. These diffusion coefficients are widely used in reconstructing the geochemistry of sedimentary formations (1,2) and in predicting the performance of natural or engineered contaminant barrier systems (3,4), radioactive waste repositories (5,6), and CO 2 repositories (7,8).…”