Effects of chemical reactions on density-dependent fluid flow: on the numerical formulation and the development of instabilities

A three-dimensional, reactive numerical flow model is developed that couples chemical reactions with density-dependent mass transport and fluid flow. The model includes equilibrium reactions for the aqueous species, kinetic reactions between the solid and aqueous phases, and full coupling of porosity and permeability changes that result from precipitation and dissolution reactions in porous media. A one-step, global implicit approach is used to solve the coupled flow, transport and reaction equations with a fully implicit upstream-weighted control volume discretization. The Newton–Raphson method is applied to the discretized non-linear equations and a block ILU-preconditioned CGSTAB method is used to solve the resulting Jacobian matrix equations. This approach permits the solution of the complete set of governing equations for both concentration and pressure simultaneously affected by chemical and physical processes. A series of chemical transport simulations are conducted to investigate coupled processes of reactive chemical transport and density-dependent flow and their subsequent impact on the development of preferential flow paths in porous media. The coupled effects of the processes driving flow and the chemical reactions occurring during solute transport is studied using a carbonate system in fully saturated porous media. Results demonstrate that instability development is sensitive to the initial perturbation caused by density differences between the solute plume and the ambient groundwater. If the initial perturbation is large, then it acts as a “trigger” in the flow system that causes instabilities to develop in a planar reaction front. When permeability changes occur due to dissolution reactions occurring in the porous media, a reactive feedback loop is created by calcite dissolution and the mixed convective transport of the system. Although the feedback loop does not have a significant impact on plume shape, complex concentration distributions develop as a result of the instabilities generated in the flow system.