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Abstract/Summary
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<jats:p>Abstract. Dissolution and precipitation processes in reactive transport in porous media are ubiquitous in a multitude of contexts within the field of Earth sciences. In particular, the dynamic interaction between the reactive dissolution and precipitation processes and the solute transport is of interest as it is capable of giving rise to the emergence of preferential flow paths in the porous host matrix. It has been shown that the emergence of preferential flow paths can be considered to be a manifestation of transport self-organization in porous media as these create spatial gradients that distance the system from the state of perfect mixing and allow for a faster and more efficient fluid transport through the host matrix. To investigate the dynamic feedback between the transport and the reactive processes in the field and its influence on the emergence of transport self-organization, we consider a two-dimensional Darcy-scale formulation of a reactive-transport setup, where the precipitation and dissolution of the host matrix are driven by the injection of an acid compound, establishing local equilibrium with the resident fluid and an initially homogeneous porous matrix, composed of a calcite mineral. The coupled reactive process is simulated in a series of computational analyses employing the Lagrangian particle-tracking (LPT) approach, capable of capturing the subtleties of the multiple-scale heterogeneity phenomena. We employ the Shannon entropy to quantify the emergence of self-organization in the field, which we define as a relative reduction in entropy compared to its maximum value. Scalability of the parameters, which characterize the evolution of the reactive process, with the Peclet number in an initially homogeneous field is derived using a simple one-dimensional ADRE model with a linear adsorption reaction term and is then confirmed through numerical simulations, with the global reaction rate, the mean value, and the variance of the hydraulic-conductivity distribution in the field all exhibiting dependency on the reciprocal of the Peclet number. Our findings show that transport self-organization in an initially homogeneous field increases with time, along with the emergence of the field heterogeneity due to the interaction between the transport and reactive processes. By studying the influence of the Peclet number on the reactive process, we arrive at a conclusion that self-organization is more pronounced in diffusion-dominated flows, characterized by small Peclet values. The self-organization of the breakthrough curve exhibits the opposite tendencies, which are observed from the perspective of a thermodynamic analogy. The hydraulic power, required to maintain the driving head pressure difference between the inlet and outlet of the field, was shown to increase with the increasing variance, as well as with the increasing mean value of the hydraulic-conductivity distribution in the field, using a simple analytic model. This was confirmed by numerical experiments. This increase in power, supplied to the flow in the field, results in an increase in the level of transport self-organization. Employing a thermodynamic framework to investigate the dynamic reaction–transport interaction in porous media may prove to be beneficial whenever the need exists to establish relations between the intensification of the preferential flow path phenomenon, represented by a decline in the Shannon entropy of the transport, with the amount of reaction that occurred in the porous medium and the change in its heterogeneity.
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