Pore-Scale Modeling of Mineral Growth and Nucleation in Reactive Flow

A fundamental understanding of mineral precipitation kinetics relies largely on microscopic observations of the dynamics of mineral surfaces exposed to supersaturated solutions. Deconvolution of tightly bound transport, surface reaction, and crystal nucleation phenomena still remains one of the main challenges. Particularly, the influence of these processes on texture and morphology of mineral precipitate remains unclear. This study presents a coupling of pore-scale reactive transport modeling with the Arbitrary Lagrangian-Eulerian approach for tracking evolution of explicit solid interface during mineral precipitation. It incorporates a heterogeneous nucleation mechanism according to Classical Nucleation Theory which can be turned “on” or “off.” This approach allows us to demonstrate the role of nucleation on precipitate texture with a focus at micrometer scale. In this work precipitate formation is modeled on a 10 micrometer radius particle in reactive flow. The evolution of explicit interface accounts for the surface curvature which is crucial at this scale in the regime of emerging instabilities. The results illustrate how the surface reaction and reactive fluid flow affect the shape of precipitate on a solid particle. It is shown that nucleation promotes the formation of irregularly shaped precipitate and diminishes the effect of the flow on the asymmetry of precipitation around the particle. The observed differences in precipitate structure are expected to be an important benchmark for reaction-driven precipitation in natural environments.

Flood generation: process patterns from the raindrop to the ocean

This article reviews river flood generation processes and flow paths across space scales. The scale steps include the pore, profile, hillslope, catchment, regional and continental scales, representing a scale range of a total of 10 orders of magnitude. Although the processes differ between the scales, there are notable similarities. At all scales, there are media patterns that control the flow of water, and are themselves influenced by the flow of water. The processes are therefore not spatially random (as in thermodynamics) but organised, and preferential flow is the rule rather than the exception. Hydrological connectivity, i.e. the presence of coherent flow paths, is an essential characteristic at all scales. There are similar controls on water flow and thus on flood generation at all scales, however, with different relative magnitudes. Processes at lower scales affect flood generation at the larger scales not simply as a multiple repetition of pore scale processes, but through interactions, which cause emergent behaviour of process patterns. For this reason, when modelling these processes, the scale transitions need to be simplified in a way that reflects the relevant structures (e.g. connectivity) and boundary conditions (e.g. groundwater table) at each scale. In conclusion, it is argued that upscaling as the mere multiple application of small scale process descriptions will not capture the larger scale patterns of flood generation. Instead, there is a need to learn from observed patterns of flood generation processes at all spatial scales.

Pore Scale Numerical Modelling of Geological Carbon Storage Through Mineral Trapping Using True Pore Geometries

Mineral trapping (MT)is the most secure method of sequestering carbon for geologically significant periods of time. The processes behind MT fundamentally occur at the pore scale, therefore understanding which factors control MT at this scale is crucial. We present a finite elements advection–diffusion–reaction numerical model which uses true pore geometry model domains generated from $$\upmu$$ μ CT imaging. Using this model, we investigate the impact of pore geometry features such as branching, tortuosity and throat radii on the distribution and occurrence of carbonate precipitation in different pore networks over 2000 year simulated periods. We find evidence that a greater tortuosity, greater degree of branching of a pore network and narrower pore throats are detrimental to MT and contribute to the risk of clogging and reduction of connected porosity. We suggest that a tortuosity of less than 2 is critical in promoting greater precipitation per unit volume and should be considered alongside porosity and permeability when assessing reservoirs for geological carbon storage (GCS). We also show that the dominant influence on precipitated mass is the Damköhler number, or reaction rate, rather than the availability of reactive minerals, suggesting that this should be the focus when engineering effective subsurface carbon storage reservoirs for long term security. Article Highlights The rate of reaction has a stronger influence on mineral precipitation than the amount of available reactant. In a fully connected pore network preferential flow pathways still form which results in uneven precipitate distribution. A pore network tortuosity of <2 is recommended to facilitate greater carbon mineralisation.