The Interplay Between Pore‐Scale Heterogeneity, Surface Roughness, and Wettability Controls Trapping in Two‐Phase Fluid Displacement in Porous Media

Predicting the compactness of the invasion front and the amount of trapped fluid left behind is of crucial importance to applications ranging from microfluidics and fuel cells to subsurface storage of carbon and hydrogen. We examine the interplay of wettability, macro‐ and pore scale heterogeneity (pore angularity and pore wall roughness), and its influence on flow patterns formation and trapping efficiency in porous media by a combination of 3D micro‐CT imaging with 2D direct visualization of micromodels. We observe various phase transitions between the following capillary flow regimes (phases): (a) compact advance, (b) wetting and drainage Invasion percolation, (c) Ordinary percolation

Membrane Based Measurement Technology for in situ Monitoring of Gases in Soil

The representative measurement of gas concentration and fluxes in heterogeneous soils is one of the current challenges when analyzing the interactions of biogeochemical processes in soils and global change. Furthermore, recent research projects on CO2-sequestration have an urgent need of CO2-monitoring networks. Therefore, a measurement method based on selective permeation of gases through tubular membranes has been developed. Combining the specific permeation rates of gas components for a membrane and Dalton's principle, the gas concentration (or partial pressure) can be determined by the measurement of physical quantities (pressure or volume) only. Due to the comparatively small permeation constants of membranes, the influence of the sensor on its surrounding area can be neglected. The design of the sensor membranes can be adapted to the spatial scale from the bench scale to the field scale. The sensitive area for the measurement can be optimized to obtain representative results. Furthermore, a continuous time-averaged measurement is possible where the time for averaging is simply controlled by the wall-thickness of the membrane used. The measuring method is demonstrated for continuous monitoring of O2 and CO2 inside of a sand filled Lysimeter. Using three sensor planes inside the sand pack, which were installed normal to the gas flow direction and a reference measurement system, we demonstrate the accuracy of the gas-detection for different flux-based boundary conditions

Quantification of capillary trapping of gas clusters using X-ray microtomography

A major difficulty in modeling multiphase flow in porous media is the emergence of trapped phases. Our experiments demonstrate that gas can be trapped in either single-pores, multipores, or in large connected networks. These large connected clusters can comprise up to eight grain volumes and can contain up to 50% of the whole trapped gas volume. About 85% of the gas volume is trapped by multipore gas clusters. This variety of possible trapped gas clusters of different shape and volume will lead to a better process understanding of bubble-mediated mass transfer. Since multipore gas bubbles are in contact with the solid surface through ultrathin adsorbed water films the interfacial area between trapped gas clusters and intergranular capillary water is only about 80% of the total gas surface. We could derive a significant (R²=0.98) linear relationship between the gas-water-interface and gas saturation. We found no systematic dependency of the front velocity of the invading water phase in the velocity range from 0.1 to 0.6 cm/min corresponding to capillary numbers from 2 x 10⁻⁷ to 10⁻⁶. Our experimental results indicate that the capillary trapping mechanism is controlled by the local pore structure and local connectivity and not by thermodynamics, i.e., by the minimum of the Free Energy, at least in the considered velocity range. Consistent with this physical picture is our finding that the trapping frequency (= bubble-size distribution) reflects the pore size distribution for the whole range of pore radii, i.e., the capillary trapping process is determined by statistics and not by thermodynamics.Keywords: gas clusters, interfacial area, capillary trappin

A New Phase Diagram for Fluid Invasion Patterns as a Function of Pore‐Scale Heterogeneity, Surface Roughness, and Wettability

Understanding how different flow patterns emerge at various macro‐ and pore scale heterogeneity,pore wettability and surface roughness is remains a long standing scientific challenge. Such understandingallows to predict the amount of trapped fluid left behind, of crucial importance to applications ranging frommicrofluidics and fuel cells to subsurface storage of carbon and hydrogen. We examine the interplay ofwettability and pore‐scale heterogeneity including both pore angularity and roughness, by a combination ofmicro‐CT imaging of 3D grain packs with direct visualization of 2D micromodels. The micromodels aredesigned to retain the key morphological and topological properties derived from the micro‐CT images.Different manufacturing techniques allow us to control pore surface roughness. We study the competitionbetween flow through the pore centers and flow along rough pore walls and corners in media of increasingcomplexity in the capillary flow regime. The resulting flow patterns and their trapping efficiency are in excellentagreement with previous μ‐CT results. We observe different phase transitions between the following flowregimes (phases): (a) Frontal/compact advance, (b) wetting and drainage Invasion percolation, and (c) Ordinarypercolation. We present a heterogeneity‐wettability‐roughness phase diagram that predicts these regimes

Evaporation Study for Real Soils Based on HYPROP Hydraulic Functions and Micro-CT-Measured Pore-Size Distribution

Evaporation—a key process for water exchange between soil and atmosphere—is controlled by convective and diffusive surface fluxes that determine the functional time dependence of the evaporation rate (). Recent studies demonstrated that only a pore-scale surface flux model can capture the correct () curve. These studies also showed that a realistic estimate of the hydraulically connected region (HCR) of the pore-size distribution (PSD) is crucial for coupling surface flux to internal water flux. Since previous studies were often based on natural sands and glass beads, the main focus of our study was to test these conclusions for real soils. Therefore, we investigated the evaporation process within undisturbed soil columns of a sandy soil and loamy sand and measured the hydraulic functions via HYPROP experiments (a system to measure hydraulic properties using the evaporation method). Based on the isolated pore evaporation (IPE) model using a discretized form of the PSD, we developed a continuous IPE model and applied it to our experiments. Because the PSD plays a central role in the IPE model, we determined the PSD of the loamy sand soil via X-ray microtomography (μCT) for pores >19 μm. The consistency of the experimental data, i.e., (i) the retention curve for deriving the HCR of the pore size distribution, (ii) the unsaturated hydraulic conductivity for calculating the characteristic lengths of the evaporation process, and (iii) the high accuracy of the mass loss data strongly support the HYPROP method for this kind of complex evaporation experiment. The continuous IPE model describes the characteristic Stage 1 behavior well (functional form of the evaporation rate and length of Stage 1) for both soil types if a realistic HCR estimate is used that (i) is derived from a characteristic length analysis estimating the lower boundary of the HCR and (ii) the upper range of the HCR is based on the true PSD derived from μCT data

Absorption and diffusion process at the CO₂-decane interface considering density fluctuations near the critical CO₂ point

Based on a new conceptual model, which considers CO2 density fluctuations in the critical range, we were able to consistently explain the time dependence of the volume increase for the respective thermodynamic state. The experimental results confirm the new conceptual model that volume swelling in the non-critical pressure range (surface effect with limited penetration depth.</p

SchlüterSteffenChemBioEnvEngineeringQuantificationCapillaryTrapping.pdf

A major difficulty in modeling multiphase flow in porous media is the emergence of trapped phases. Our experiments demonstrate that gas can be trapped in either single-pores, multipores, or in large connected networks. These large connected clusters can comprise up to eight grain volumes and can contain up to 50% of the whole trapped gas volume. About 85% of the gas volume is trapped by multipore gas clusters. This variety of possible trapped gas clusters of different shape and volume will lead to a better process understanding of bubble-mediated mass transfer. Since multipore gas bubbles are in contact with the solid surface through ultrathin adsorbed water films the interfacial area between trapped gas clusters and intergranular capillary water is only about 80% of the total gas surface. We could derive a significant (R²=0.98) linear relationship between the gas-water-interface and gas saturation. We found no systematic dependency of the front velocity of the invading water phase in the velocity range from 0.1 to 0.6 cm/min corresponding to capillary numbers from 2 x 10⁻⁷ to 10⁻⁶. Our experimental results indicate that the capillary trapping mechanism is controlled by the local pore structure and local connectivity and not by thermodynamics, i.e., by the minimum of the Free Energy, at least in the considered velocity range. Consistent with this physical picture is our finding that the trapping frequency (= bubble-size distribution) reflects the pore size distribution for the whole range of pore radii, i.e., the capillary trapping process is determined by statistics and not by thermodynamics.Keywords: gas clusters, interfacial area, capillary trappingKeywords: gas clusters, interfacial area, capillary trappin

SchlüterSteffenChemBioEnvEngineeringQuantificationCapillaryTrapping_SupplementaryMaterial.pdf

A major difficulty in modeling multiphase flow in porous media is the emergence of trapped phases. Our experiments demonstrate that gas can be trapped in either single-pores, multipores, or in large connected networks. These large connected clusters can comprise up to eight grain volumes and can contain up to 50% of the whole trapped gas volume. About 85% of the gas volume is trapped by multipore gas clusters. This variety of possible trapped gas clusters of different shape and volume will lead to a better process understanding of bubble-mediated mass transfer. Since multipore gas bubbles are in contact with the solid surface through ultrathin adsorbed water films the interfacial area between trapped gas clusters and intergranular capillary water is only about 80% of the total gas surface. We could derive a significant (R²=0.98) linear relationship between the gas-water-interface and gas saturation. We found no systematic dependency of the front velocity of the invading water phase in the velocity range from 0.1 to 0.6 cm/min corresponding to capillary numbers from 2 x 10⁻⁷ to 10⁻⁶. Our experimental results indicate that the capillary trapping mechanism is controlled by the local pore structure and local connectivity and not by thermodynamics, i.e., by the minimum of the Free Energy, at least in the considered velocity range. Consistent with this physical picture is our finding that the trapping frequency (= bubble-size distribution) reflects the pore size distribution for the whole range of pore radii, i.e., the capillary trapping process is determined by statistics and not by thermodynamics.Keywords: interfacial area, gas clusters, capillary trappingKeywords: interfacial area, gas clusters, capillary trappin

The Impact of Wettability and Surface Roughness on Fluid Displacement and Capillary Trapping in 2-D and 3-D Porous Media: 2. Combined Effect of Wettability, Surface Roughness, and Pore Space Structure on Trapping Efficiency in Sand Packs and Micromodels

A comprehensive understanding of the combined effects of surface roughness and wettability on the dynamics of the trapping process is lacking. This can be primarily attributed to the contradictory experimental and numerical results regarding the impact of wettability on the capillary trapping efficiency. The discrepancy is presumably caused by the surface roughness of the inner pore-solid interface. Herein, we present a comparative μ-CT study of the static fluid-fluid pattern in porous media with smooth (glass beads) and rough surfaces (natural sands). For the first time, a global optimization method was applied to map the characteristic geometrical and morphological properties of natural sands to 2-D micromodels that exhibit different degrees of surface roughness. A realistic wetting model that describes the apparent contact angle of the rough surface as a function surface morphology and the intrinsic contact angle was also proposed. The dynamics of the trapping processes were studied via visualization micromodel experiments. Our results revealed that sand and glass beads displayed opposite trends in terms of the contact angle dependence between 5° and 115°. Sand depicted a nonmonotonous functional contact angle dependency, that is, a transition from maximal trapping to no trapping, followed by an increase to medium trapping. In contrast, glass beads showed a sharp transition from no trapping to maximal trapping. Since both porous media exhibit similar morphological properties (similar Minkowski functions: porosity, surface density, mean curvature density, Euler number density), we deduce that this difference in behavior is caused by the difference in surface roughness that allows complete wetting and hence precursor thick-film flow for natural sands. Experimental results on micromodels verified this hypothesis