Pore-scale Processes Research Articles

State of the Art on Fe Precipitation in Porous Media: Hydrogeochemical Processes and Evolving Parameters

The mixing of terrestrial groundwater and seawater creates dynamic reaction zones in intertidal areas, where land-derived Fe(II) is oxidized to Fe(III) and then precipitates as Fe hydroxides at the groundwater–seawater interface. These hydrogeochemical processes contribute to the formation of iron bands at the saltwater wedge (SW) and beneath the upper saline plume (USP). This study provides a comprehensive review of physical and geochemical processes at field scale in coastal areas, explores the impact of mineral precipitation on pore structure at pore scale, and synthesizes reactive transport modeling (RTM) approaches for illustrating continuum-scale soil physio-chemical parameters during the evolution of porous media. Upon this review, knowledge gaps and research needs are identified. Additionally, challenges and opportunities are presented. Therefore, we reach the conclusion that the incorporation of observational data into a comprehensive physico-mathematical model becomes imperative for capturing the pore-scale processes in porous media and their influence on groundwater flow and solute transport at large scales. Additionally, a synergistic approach, integrating pore-scale modeling and non-invasive imaging, is equally essential for providing detailed insights into intricate fluid–pore–solid interactions for future studies, as well as facilitating the development of regional engineering-scale models and physio-chemical coupled models with diverse applications in marine science and engineering.

Counter-current spontaneous imbibition dynamics: Combined effects of wettability, fracture flow, and pore structure

Spontaneous imbibition plays a crucial role in various engineering and industrial applications, with its efficiency significantly influenced by a range of factors. To unravel the intricate mechanisms behind these factors, our study employs pore-scale numerical simulations. Utilizing a color gradient model within the framework of the lattice Boltzmann method, we delve into how pore structure, wettability, and flow velocity within fractures collectively impact spontaneous imbibition. Our findings reveal that the dynamics of drainage and imbibition interfaces during countercurrent spontaneous imbibition are key determinants of imbibition efficiency. Specifically, the synergy between wettability and pore structure markedly affects the penetration depth and distribution characteristics of the imbibition interface, which, in turn, influences the imbibition's speed and duration. Moreover, the interaction between the flow velocity inside fractures and the configuration of adjacent pore structures significantly shapes the evolution of the drainage interface. This interplay is crucial as it can either enhance or hinder countercurrent spontaneous imbibition. These insights deepen our understanding of the pore-scale processes governing countercurrent spontaneous imbibition, laying a solid theoretical foundation for optimizing its application in engineering and industrial settings.

Effects of displacement velocity on interfacial reconstruction events during immiscible two-phase displacement

During the two-phase fluid displacement in porous media, with the increase in capillary number Ca, different wettability effects are suppressed; however, its potential control mechanism has not been clarified. Therefore, in this study, we have analyzed the pore scale process related to interface reconfiguration events in detail and profoundly clarified the nature of a series of interface reconfiguration events being suppressed. Based on typical pore throat, we elaborated and confirmed that the development and evolution direction of fluid displacement mode always follow the principle of minimum operating power. That is to say, in order to avoid extra work, the system will compare all the potential moving meniscus at the displacement front and always choose the local path with the minimum operating power (Po=ΔpQ) of the system for displacement. Under this theory, a series of interface reconfiguration events are considered energy favorable self-regulation events derived by the system in order to avoid extra energy consumption. However, the appearance and disappearance of interface reconstruction events are considered to be the result of the mechanism of “self-regulation of surface energy change rate” and “self-regulation of viscosity dissipation rate” in order to approach the minimum operating power. This study provides us with a sufficient physical explanation to understand the nature of the wettability effect being suppressed.

A Convenient Device to Measure the Permeability of Intact Rock (Heterogeneity and Anisotropy)

Abstract The permeability of intact rocks affects a wide range of natural and engineered systems, yet its measurement remains costly and involves time demanding test protocols. Gas permeameters may improve efficiency but involve a complex series of pore-scale processes. In addition, peripheral damage during coring and the jacket-rock interface create a preferential flow path that affects the inferred permeability. We present a convenient permeameter for liquid-based permeability measurements using an unjacketed disk specimen. The test configuration minimizes peripheral flow bias and expedites testing times. The permeameter uses readily available devices for pressure and flow rate measurement/control and can be readily configured to measure rock permeability across six orders of magnitude. Preliminary numerical simulations allowed us to optimize the test design, to extract coefficients for data correction, and to process data to recover permeability anisotropy. The system is experimentally verified against industry standards and used to test cleaning protocols to remove fines left on the specimen surface after specimen preparation; these fines may cause clogging at the inlet phase—a bias that affects all permeameters.

Pore-scale characterization of residual gas remobilization in CO2 geological storage

A decrease in reservoir pressure can lead to remobilization of residually trapped CO2. In this study, the pore-scale processes related to trapped CO2 remobilization under pressure depletion were investigated with the use of high-resolution 3D X-ray microtomography. The distribution of CO2 in the pore space of Bentheimer sandstone was measured after waterflooding at a fluid pressure of 10 MPa, and then at pressures of 8, 6 and 5 MPa. At each stage CO2 was produced, implying that swelling of the gas phase and exsolution allowed the gas to reconnect and flow. After production, the gas reached a new position of equilibrium where it may be trapped again. At the end of the experiment, we imaged the sample again after 30 hours. Firstly, the results showed that an increase in saturation beyond the residual value was required to remobilize the gas, which is consistent with earlier field-scale results. Additionally, Ostwald ripening and continuing exsolution lead to a significant change in fluid saturation: transport of dissolved gas in the aqueous phase to equilibriate capillary pressure led to reconnection of the gas and its flow upwards under gravity. The implications for CO2 storage are discussed: an increase in saturation beyond the residual value is required to mobilize the gas, but Ostwald ripening can allow local reconnection of hitherto trapped gas, thus enhancing migration and may reduce the amount of CO2 that can be capillary trapped in storage operations.

Advanced Digital-SCAL Measurements of Gas Trapped in Sandstone

Trapped gas saturation (Sgr) plays an important role in subsurface engineering, such as carbon capture and storage, H2 storage efficiency as well as the production of natural gas. Unfortunately, Sgr is notoriously difficult to measure in the laboratory or field. The conventional method of measurement—low-rate unsteady-state coreflooding—is often impacted by gas dissolution effects, resulting in large uncertainties of the measured Sgr. Moreover, it is not understood why this effect occurs, even for brines carefully pre-equilibrated with gas. To address this question, we used high-resolution X-ray computed tomography (micro-CT) imaging techniques to directly visualize the pore-scale processes during gas trapping. Consistent with previous studies, we find that for pre-equilibrated brine, the remaining gas saturation continually decreased with more (pre-equilibrated) brine injected and even after the brine injection was stopped, resulting in very low Sgr values (possibly even zero) at the pore-scale level. Furthermore, we were able to clearly observe the initial trapping of gas by the snap-off effect, followed by a further shrinkage of the gas clusters that had no connected pathway to the outside. Our experimental insights suggest that the effect is related to the effective phase behavior of gas inside the porous medium, which due to the geometric confinement, could be different from the phase behavior of bulk fluids. The underlying mechanism is likely linked to ripening dynamics, which involves a coupling between phase equilibrium and dissolution/partitioning of components, diffusive transport, and capillarity in the geometric confinement of the pore space.

How nanoporous silicon-polypyrrole hybrids flex their muscles in aqueous electrolytes: In operando high-resolution x-ray diffraction and electron tomography-based micromechanical computer simulations

Macroscopic strain experiments revealed that Si crystals traversed by parallel, channel-like nanopores functionalized with the muscle polymer polypyrrole exhibit large and reversible electrochemo-mechanical actuation in aqueous electrolytes. On the microscopical level this system still bears open questions, as to how the electrochemical expansion and contraction of PPy acts on to np-Si pore walls and how the collective motorics of the pore array emerges from the single-nanopore behavior. An analysis of in operando X-ray diffraction experiments with micromechanical finite element simulations, based on a 3D reconstruction of the nanoporous medium by TEM tomography, shows that the in-plane mechanical response is dominantly isotropic despite the anisotropic elasticity of the single crystalline host matrix. However, the structural anisotropy originating from the parallel alignment of the nanopores lead to significant differences between the in- and out-of-plane electromechanical response. This response is not describable by a simple 2D arrangement of parallel cylindrical channels. Rather, the simulations highlight that the dendritic shape of the Si pore walls, including pore connections between the main channels, cause complex, inhomogeneous stress-strain fields in the crystalline host. Time-dependent X-ray scattering on the dynamics of the actuator properties hint towards the importance of diffusion limitations, plastic deformation and creep in the nanoconfined polymer upon (counter-)ion adsorption and desorption, the very pore-scale processes causing the macroscopic electroactuation. From a more general perspective, our study demonstrates that the combination of TEM tomography-based micromechanical modeling with high-resolution X-ray scattering experiments provides a powerful approach for in operando analysis of nanoporous composites from the single-nanopore up to the porous-medium scale.

How interfacial dynamics controls drainage pore-invasion patterns in porous media

Immiscible two-phase flow through porous media is composed of a series of pore invasions; however, the consequences of pore-scale processes on macroscopic fluid front behavior remain to be clarified. In this work, we perform an analytical and experimental investigation of front behavior and pore invasions dynamics during drainage for various viscosity ratios and capillary numbers. We use a microfluidic setup that includes a fully controlled pore-doublet geometry to isolate and explore pore-invasion mechanisms. We apply a model based on volume-averaged Navier–Stokes equations to capture interface dynamics. Different invasion mechanisms are characterized and correlated with front behavior for various flow conditions. For the viscous flow regime, a succession of continuous pore invasions is observed, leaving a thick layer of wetting phase behind at pore curvatures. Abrupt interfacial jumps, followed by an apparent stagnant condition, are observed for the capillary flow regime. We identified a new regime, called crossover flow regime, for which pore invasion shows a mixed behavior between capillary and viscous dominated regimes. The global front behavior is predicted based on the numerical simulation and experimental results for all flow regimes.

Pore-scale visualization of hydrogen storage in a sandstone at subsurface pressure and temperature conditions: Trapping, dissolution and wettability

HypothesisUnderground hydrogen (H2) storage is a potentially viable solution for large-scale cyclic H2 storage; however, the behavior of H2 at subsurface pressure and temperature conditions is poorly known. This work investigates if the pore-scale displacement processes in H2-brine systems in a porous sandstone can be sufficiently well defined to enable effective and economic storage operations. In particular, this study investigates trapping, dissolution, and wettability of H2-brine systems at the pore-scale, at conditions that are realistic for subsurface H2 storage. ExperimentsWe have performed in situ X-ray imaging during a flow experiment to investigate pore-scale processes during H2 injection and displacement in a brine saturated Bentheimer sandstone sample at temperature and pressure conditions representative of underground reservoirs. Two injection schemes were followed for imbibition: displacement of H2 with H2-equilibrated brine and with non-H2-equilibrated brine. The results from the two cycles were compared with each other. FindingsThe sandstone was found to be wetting to the brine and non-wetting to H2 after both displacement cycles, with average contact angles of 54° and 53° for H2-equilibrated and non-H2-equilibrated brine respectively. We also found a higher recovery of H2 (43.1%) when displaced with non-H2-equilibrated brine compared to that of H2-equilibrated brine (31.6%), indicating potential dissolution of H2 in the unequilibrated imbibing brine at reservoir conditions. Our results suggest that underground H2 storage may indeed be a suitable strategy for energy storage, but considerable further research is needed to fully comprehend the pore-scale interactions at reservoir conditions.

Investigation on reactive flow through porous media by quadtree Lattice Boltzmann

In this study, in order to investigate the effect of the underlying pore-scale processes on continuum scale simulations of porous media dissolution, we improve the standard Lattice Boltzmann method using Quadtree grid refinement approach to simulate fluid flow and reactive transport through large domain sizes. Our results have shown considerable computational improvements up to 80% in simulation time together with increased numerical accuracy. The results and the added value of the new approach are discussed using comparison of our model with the conventional LBM. Moreover, we have applied a systematic analysis by increasing complexity levels and starting from fluid flow and continuing with tracer transport and reactive transport in single pores, and ultimately, reactive transport in dissolving porous structures. For each case, the accuracy and computational benefits of the Quadtree models are discussed and dimensionless numbers are used to characterize regimes of flow and reaction in each step of comparison. Porosity-permeability variation in a 2D pore structure and mass transfer coefficient in a closed-end fracture with porous walls are then evaluated under different flow conditions.

Pore-Scale Wetting Process of Capillary-Driven Flow in Unsaturated Porous Media under Micro- and Earth-Gravities

Microgravity hinders capillary-driven water flow in unsaturated porous media. Previous studies proposed pore-scale phenomena such as “air entrapment”, “particle separation”, and “interruption on widening void space” to explain gravity-dependent capillary-driven flows. Our objectives were: (1) to measure the water flux densities of the pore-scale capillary-driven flow in micro- and Earth-gravities and (2) to reveal that what makes water flow slower under microgravity than under 1 G. We found that average macroscopic water flux densities had no significant difference under micro- and Earth-gravities (p = 0.30). We did not observe “air entrapment” in the pore spaces of porous media. “Widening on a single particle” and “capillary widening” disturbed capillary-driven flow; however, “widening on a single particle” had no significant gravity dependency. “Capillary widening” may be independent of gravity, since it was observed both under microgravity and under 1 G. Water flux densities in unsaturated porous media may have gravity dependency induced by “particle separation” only when porosity is large enough to allow particles to move.

Pore-scale processes in tertiary low salinity waterflooding in a carbonate rock: Micro-dispersions, water film growth, and wettability change

HypothesisThe wettability change from oil-wet towards more water-wet conditions by injecting diluted brine can improve oil recovery from reservoir rocks, known as low salinity waterflooding. We investigated the underlying pore-scale mechanisms of this process to determine if improved recovery was associated with a change in local contact angle, and if additional displacement was facilitated by the formation of micro-dispersions of water in oil and water film swelling. ExperimentsX-ray imaging and high-pressure and temperature flow apparatus were used to investigate and compare high and low salinity waterflooding in a carbonate rock sample. The sample was placed in contact with crude oil to obtain an initial wetting state found in hydrocarbon reservoirs. High salinity brine was then injected at increasing flow rates followed by low salinity brine injection using the same procedure. FindingsDevelopment of water micro-droplets within the oil phase and detachment of oil layers from the rock surface were observed after low salinity waterflooding. During high salinity waterflooding, contact angles showed insignificant changes from the initial value of 115°, while the mean curvature and local capillary pressure values remained negative, consistent with oil-wet conditions. However, with low salinity, the decrease in contact angle to 102° and the shift in the mean curvature and capillary pressure to positive values indicate a wettability change. Overall, our analysis captured the in situ mechanisms and processes associated with the low salinity effect and ultimate increase in oil recovery.

Flood generation: process patterns from the raindrop to the ocean

Abstract. 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 organized, 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 but with different relative magnitudes. Processes at lower scales affect flood generation at 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.

Wicking dynamics in yarns

The spontaneous imbibition of a liquid within porous media, known as wicking, can display uncommon features in textiles and yarns. Yarns exhibited step-wise wicking dynamics not captured by current models. HypothesisWicking dynamics in yarns not only depend on inter-fiber pore filling, but are mainly determined by the pore-to-pore transition processes and the structure of the pore network. ExperimentsFast X-ray tomographic microscopy is employed to reveal the pore scale processes and neutron radiography for the macroscopic water uptake in yarns. A semi-empirical pore network model is presented that employs the measured pore network topology and pore scale dynamics to reproduce the experimentally observed wicking dynamics in yarns. FindingsThe yarn pore system is a sparse network of long and narrow pores that promotes step-wise uptake dynamics. Wicking in yarns displays fast pore filling events in the order of seconds and long waiting times between filling events up to several minutes while navigating the pore network. As main result, we find that a few filling events directly determine the macroscopic behavior of wicking in the sparse pore network of yarns. It is necessary to consider pore-to-pore transition waiting times and the pore network structure to explain the characteristics of wicking dynamics in yarns.

Research on Boundary Layer Effect in Fractured Reservoirs Based on Pore-Scale Models

It is of great significance to study the seepage characteristics of heavy oil reservoirs, which are conducive to the efficient development of resources. Boundary layer effect (BLE) exists in the pore-scale flow process of macromolecular fluid media, which is different from the flow law of conventional fluid in the pore, yet the influence of BLE is ignored in the previous pore-scale simulation. Conventional porous media simulations have difficulty analyzing the mass transfer law of small-scale models under the influence of microfractures. Based on the CT scanning data and thin section data of the real core in the target area, the rock skeleton and flow space were extracted according to the maximum ball algorithm, and the pore network model representing the complex structure was constructed. The microscale effect of macromolecules in the flow process in the pores was characterized by modifying the effective flow. The effects of the BLE on the effective connectivity, displacement process, and oil distribution law were analyzed. The seepage characteristics of different wettability conditions and different water cut stages were compared. The results show that BLE reduces the effective flow space and leads to deviations in the relative permeability curve and capillary curve. For fractured porous media, the irregular shape of porous media was characterized by the morphological method, and the mass transfer process was analyzed by the equivalent flux method. The influence of the porous media shape on the macromass transfer process was compared. This study provides a solution to the problem of BLE in pore-scale simulation.

Benchmarking the Viability of 3D Printed Micromodels for Single Phase Flow Using Particle Image Velocimetry and Direct Numerical Simulations

Holistic understanding of multiphase reactive flow mechanisms such as CO2 dissolution, multiphase displacement, and snap-off events is vital for optimisation of large-scale industrial operations like CO2 sequestration, enhanced oil recovery, and geothermal energy. Recent advances in three-dimensional (3D) printing allow for cheap and fast manufacturing of complex porosity models, which enable investigation of specific flow processes in a repeatable manner as well as sensitivity analysis for small geometry alterations. However, there are concerns regarding dimensional fidelity, shape conformity and surface quality, and therefore, the printing quality and printer limitations must be benchmarked. We present an experimental investigation into the ability of 3D printing to generate custom-designed micromodels accurately and repeatably down to a minimum pore-throat size of 140 μm, which is representative of the average pore-throat size in coarse sandstones. Homogeneous and heterogeneous micromodel geometries are designed, then the 3D printing process is optimised to achieve repeatable experiments with single-phase fluid flow. Finally, Particle Image Velocimetry is used to compare the velocity map obtained from flow experiments in 3D printed micromodels with the map generated with direct numerical simulation (OpenFOAM software) and an accurate match is obtained. This work indicates that 3D printed micromodels can be used to accurately investigate pore-scale processes present in CO2 sequestration, enhanced oil recovery and geothermal energy applications more cheaply than traditional micromodel methods.

New type of pore-snap-off and displacement correlations in imbibition

HypothesisImbibition of a fluid into a porous material involves the invasion of a wetting fluid in the pore space through piston-like displacement, film and corner flow, snap-off and pore bypassing. These processes have been studied extensively in two-dimensional (2D) porous systems; however, their relevance to three-dimensional (3D) natural porous media is poorly understood. Here, we investigate these pore-scale processes in a natural rock sample using time-resolved 3D (i.e., four-dimensional or 4D) X-ray imaging. ExperimentsWe performed a capillary-controlled drainage-imbibition experiment on an initially brine-saturated carbonate rock sample. The sample was imaged continuously during imbibition using 4D X-ray imaging to visualize and analyze fluid displacement and snap-off processes at the pore-scale. FindingsWe discover a new type of snap-off that occurs in pores, resulting in the entrapment of a small portion of the non-wetting phase in pore corners. This contrasts with previously-observed snap-off in throats which traps the non-wetting phase in pore centers. We relate the new type of pore-snap-off to the pinning of fluid–fluid interfaces at rough surfaces, creating contact angles close to 90°. Subsequently, we provide correlations for displacement events as a function of pore-throat geometry. Our findings indicate that having a small throat does not necessarily favor snap-off: the key criterion is the throat radius in relation to the pore radius involved in a displacement event, captured by the aspect ratio.

Combining innovative experimental approaches and cross-scale reactive transport modelling for assessing coupled hydrogeochemical processes at interfaces in deep geological repositories for radioactive waste

Abstract. Deep geological repositories with a multi-barrier concept are foreseen by various countries for the disposal of high-level radioactive waste. A reliable and consistent assessment of the safety of these repositories over time scales of some hundred thousand years requires an advancement of process understanding. Simulation tools need to be developed for a close-to-reality description of repository evolution scenarios. This is especially required to resolve the challenging task of comparing and assessing the safety of different repository concepts in different host rocks within the German site-selection process. The construction of underground galleries and geotechnical barriers in the host rock formation and the emplacement of nuclear waste packages will create perturbations induced by chemical, thermal and pressure gradients at the interfaces of the different barriers, leading to mineral dissolution and precipitation to achieve re-equilibration. Such coupled hydrogeochemical processes generate non-linear responses in transport and mechanical properties of barrier materials and host rocks, which have to be taken into account for a more rigorous assessment of repository system evolution. Reactive transport modeling (RTM) can be applied to investigate these perturbations and processes across temporal and spatial scales, from the micro-scale at interfaces via the repository near field to the entire repository system – information not accessible through experiments alone. Although RTM is capable of addressing highly complex hydrogeochemical phenomena, the application of RTM codes to real systems is impeded by the often simplified description of coupled processes. To enhance the predictive capabilities of reactive transport models and to gain fundamental insights into the coupling between solute and radionuclide transport properties (e.g., permeability and diffusivity) of porous media and dissolution/precipitation processes, we conducted experiments on “simplified” chemical systems combined with pore-scale and continuum-scale reactive transport modelling to study processes in isolation, with the final aim of improving conceptual approaches for process couplings implemented in reactive transport codes. In this context, we investigated the effects of coupled mineral dissolution and precipitation in porous media on changes in permeability using flow-through experiments conducted in a magnetic resonance imaging scanner, which enabled the in situ investigation of porosity evolution in combination with monitoring changes in permeability and mineralogy. Our observations showed that classical implementations in reactive transport codes such as the Kozeny–Carman equation (Carman, 1937) failed to reproduce the changes in permeability and that more sophisticated approaches are required (Poonoosamy et al., 2020a, b). Moreover, we developed a novel “lab-on-a-chip” setup, i.e., micronized counter diffusion reactors with in operando 3D Raman tomography (Poonoosamy et al., 2019, 2020c), which enables evaluation of the alteration in pore architecture and study of the effect of coupled mineral dissolution and precipitation on the diffusive transport of solutes and radionuclides in porous media. Our approach enables the development of process-based theoretical models which allow for improvements in RTM codes and for predicting the evolution of perturbed interfaces in waste repositories, thus building confidence in the predictive capabilities of reactive transport models and reducing uncertainties with respect to future repository evolution.

Rain, Snow and Frozen Soil: Open Questions from a Porescale Perspective with Implications for Geohazards

Climate change is already affecting high mountain regions, such as the European Alps. Those regions will be confronted with a significant rise of temperatures above the global average, and more and heavier rain events, also during wintertime. The system response to the coincidence of rain, snow, and possibly frozen soil depends on the almost infinite number of possible combinations of thermo-hydraulic states of the involved phases. Landslides, snow avalanches, debris flows, or extensive surface runoff are just a few of the possible hazardous outcomes. With rising temperatures and increased precipitation, those hazardous outcomes are expected to occur even more frequently in the future, requiring a better understanding of those coupled processes for hazard mitigation strategies. The macroscopic phenomena are controlled by porescale processes, such as water freezing and ice grains blocking pores, which are only barely understood. The strong coupling between thermal state and hydraulic parameters, the possible phase change, and material heterogeneity pose great challenges for investigation. This work provides an overview of documented hazard events regarding rain, snow, and possibly frozen soil. The current state in theoretical and experimental research is presented before several knowledge gaps are derived and possible techniques to address those gaps are discussed.

Probabilistic nucleation governs time, amount, and location of mineral precipitation and geometry evolution in the porous medium

One important unresolved question in reactive transport is how pore-scale processes can be upscaled and how predictions can be made on the mutual effect of chemical processes and fluid flow in the porous medium. It is paramount to predict the location of mineral precipitation besides their amount for understanding the fate of transport properties. However, current models and simulation approaches fail to predict precisely where crystals will nucleate and grow in the spatiotemporal domain. We present a new mathematical model for probabilistic mineral nucleation and precipitation. A Lattice Boltzmann implementation of the two-dimensional mineral surface was developed to evaluate geometry evolution when probabilistic nucleation criterion is incorporated. To provide high-resolution surface information on mineral precipitation, growth, and distribution, we conducted a total of 27 calcium carbonate synthesis experiments in the laboratory. The results indicate that nucleation events as precursors determine the location and timing of crystal precipitation. It is shown that reaction rate has primary control over covering the substrate with nuclei and, subsequently, solid-phase accumulation. The work provides insight into the spatiotemporal evolution of porous media by suggesting probabilistic and deterministic domains for studying reactive transport processes. We indicate in which length- and time-scales it is essential to incorporate probabilistic nucleation for valid predictions.