Crystal surface reactivity analysis using a combined approach of X-ray micro-computed tomography and vertical scanning interferometry

Kahl, Wolf‐Achim; Tao, Yuan; Bollermann, Till; Bach, Wolfgang

doi:10.2475/01.2020.03

Cited by 14 publications

(24 citation statements)

References 83 publications

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“…The second consists in computing the 3D distance field, also called distance map or distance function, on a reference volume, starting from the interface which constitutes a zero level set, and looking at the intercept of the distance map with the interface at another time step. Both methods are convenient to further measure the interface displacement rate or the reaction rate, as already shown in studies focusing on dissolution of fracture walls [100], mini-boreholes [66] or minerals [100,109,108,160] or precipitation in porous media [112].…”

Section: Evaluation Of Displacement and Local Reaction Rates For Evolving Fluid-mineral Interfacesmentioning

confidence: 98%

Pore-Scale Imaging and Modelling of Reactive Flow in Evolving Porous Media: Tracking the Dynamics of the Fluid–Rock Interface

Noiriel

Soulaine

2021

Transp Porous Med

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Fluid-mineral and fluid-rock interfaces are key parameters controlling the reactivity and fate of fluids in reservoir rocks and aquifers. The interface dynamics through space and time results from complex processes involving a tight coupling between chemical reactions and transport of species as well as a strong dependence on the physical, chemical, mineralogical and structural properties of the reacting solid phases. In this article, we review the recent advances in pore-scale imaging and reactive flow modelling applied to interface dynamics. Digital rocks derived from time-lapse X-ray micro-tomography imaging gives unprecedented opportunity to track the interface evolution during reactive flow experiments in porous or fractured media, and evaluate locally mineral reactivity. The recent improvements in porescale reactive transport modelling allow for a fine description of flow and transport that integrates moving fluid-mineral interfaces inherent to chemical reactions. Combined with three-dimensional digital images, pore-scale reactive transport modelling complements and augments laboratory experiments. The most advanced multi-scale models integrate sub-voxel porosity and processes which relate to imaging instrument resolution and improve upscaling possibilities. Two example applications based on the solver porousMedia4Foam illustrate the dynamics of the interface for different transport regimes (i.e., diffusive-to advective-dominant) and rock matrix properties (i.e., permeable versus impermeable, and homogeneous versus polymineralic). These parameters affect both the interface roughness and its geometry evolution, from sharp front to smeared (i.e., diffuse) interface. The paper concludes by discussing the challenges associated with precipitation processes in porous media, rock texture and composition (i.e., physical and mineralogical heterogeneity), and upscaling to larger scales.

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Section: Evaluation Of Displacement and Local Reaction Rates For Evolving Fluid-mineral Interfacesmentioning

confidence: 98%

Pore-Scale Imaging and Modelling of Reactive Flow in Evolving Porous Media: Tracking the Dynamics of the Fluid–Rock Interface

Noiriel

Soulaine

2021

Transp Porous Med

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“…The simulated material flux was used to calculate the rate map by dividing the surface retreat by the molar volume of calcite, identical to the rate map calculations using experimental data . The rate maps consist of surface pixels representing the absolute rate values.…”

Section: Modelingmentioning

confidence: 99%

“…The reaction rate spectrum data allow to identify and quantify rate contributors, such as rate portions responsible for enhanced rates at crystal corners and edges and grain boundaries . The interferometry microscopy data sets used in this study are described in a previous experimental study, including all experimental and analytical details …”

Section: Modelingmentioning

confidence: 99%

“…They concluded that the increase of surface area due to the increase of surface roughness is the sole factor responsible for a local increase of the dissolution rate. Nevertheless, while the impact of transport heterogeneities on reaction rate variability is well established in RTM, the effect of variability of surface reactivity is less developed in numerical approaches. , …”

Section: Introductionmentioning

confidence: 99%

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Implementing Heterogeneous Crystal Surface Reactivity in Reactive Transport Simulations: The Example of Calcite Dissolution

Karimzadeh

2021

ACS Earth Space Chem.

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Both surface reactivity and fluid dynamics control the dissolution kinetics of crystalline material. In this study, we performed a 3D reactive transport simulation to investigate the impact of surface topography heterogeneity superimposed to fluid transport heterogeneity on the dissolution rate of calcite. The model simulates the chemical reaction of calcite dissolution, solute transport, and crystal surface geometry evolution. Importantly, we introduce heterogeneous surface reactivity into the reactive transport simulation. We test the surface slope factor as a proxy value for the intrinsic surface reactivity of dissolving crystal surface nanotopographies. Experimental data sets collected using vertical scanning interferometry validate this approach. The novel parametrization allows for the simulation of surface-controlled heterogeneous reactivity in reactive transport simulations of mineral surface dissolution.

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“…The rate distribution of dissolving (10-14) faces is more complex ( Brand et al 2017;Fischer et al 2012;Levenson and Emmanuel 2013). Here, comparatively low rates are locally superimposed with rate components of single etch pits as well as coalescing pits ( Fischer et al (2014); Kahl et al (2020)) that may form very reactive "super" steps (Bibi et al 2018). Consequently, we parameterize our kinetic dissolution model based on a compilation of simplified literature data, summarized in Table 2.…”

Section: Rate Componentsmentioning

confidence: 99%

Implementing the Variability of Crystal Surface Reactivity in Reactive Transport Modeling

2021

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Current reactive transport model (RTM) uses transport control as the sole arbiter of differences in reactivity. For the simulation of crystal dissolution, a constant reaction rate is assumed for the entire crystal surface as a function of chemical parameters. However, multiple dissolution experiments confirmed the existence of an intrinsic variability of reaction rates, spanning two to three orders of magnitude. Modeling this variance in the dissolution process is vital for predicting the dissolution of minerals in multiple systems. Novel approaches to solve this problem are currently under discussion. Critical applications include reactions in reservoir rocks, corrosion of materials, or contaminated soils. The goal of this study is to provide an algorithm for multi-rate dissolution of single crystals, to discuss its software implementation, and to present case studies illustrating the difference between the single rate and multi-rate dissolution models. This improved model approach is applied to a set of test cases in order to illustrate the difference between the new model and the standard approach. First, a Kossel crystal is utilized to illustrate the existence of critical rate modes of crystal faces, edges, and corners. A second system exemplifies the effect of multiple rate modes in a reservoir rock system during calcite cement dissolution in a sandstone. The results suggest that reported variations in average dissolution rates can be explained by the multi-rate model, depending on the geometric configurations of the crystal surfaces.

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Crystal surface reactivity analysis using a combined approach of X-ray micro-computed tomography and vertical scanning interferometry

Cited by 14 publications

References 83 publications

Pore-Scale Imaging and Modelling of Reactive Flow in Evolving Porous Media: Tracking the Dynamics of the Fluid–Rock Interface

Pore-Scale Imaging and Modelling of Reactive Flow in Evolving Porous Media: Tracking the Dynamics of the Fluid–Rock Interface

Implementing Heterogeneous Crystal Surface Reactivity in Reactive Transport Simulations: The Example of Calcite Dissolution

Implementing the Variability of Crystal Surface Reactivity in Reactive Transport Modeling

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