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A saturation–capillary pressure relationship is proposed that is applicable for all wettabilities, including mixed-wet and oil-wet or hydrophobic media. This formulation is more flexible than existing correlations that only match water-wet data, while also allowing saturation to be written as a closed-form function of capillary pressure: we can determine capillary pressure explicitly from saturation, and vice versa. We propose P c = A + B tan π 2 - π S e C for 0 ≤ S e ≤ 1 , where S e is the normalized saturation. A indicates the wettability: A > 0 is a water-wet medium, A < 0 is hydrophobic while small A suggests mixed wettability. B represents the average curvature and pore-size distribution which can be much lower in mixed-wet compared to water-wet media with the same pore structure if the menisci are approximately minimal surfaces. C is an exponent that controls the inflection point in the capillary pressure and the asymptotic behaviour near end points. We match the model accurately to 29 datasets in the literature for water-wet, mixed-wet and hydrophobic media, including rocks, soils, bead and sand packs and fibrous materials with over four orders of magnitude difference in permeability and porosities from 20% to nearly 90%. We apply Leverett J-function scaling to make the expression for capillary pressure dimensionless and discuss the behaviour of analytical solutions for spontaneous imbibition. [ABSTRACT FROM AUTHOR]

Three-phase flow in porous media is encountered in many applications including subsurface carbon dioxide storage, enhanced oil recovery, groundwater remediation and the design of microfluidic devices. However, the pore-scale physics that controls three-phase flow under capillary dominated conditions is still not fully understood. Recent advances in three-dimensional pore-scale imaging have provided new insights into three-phase flow. Based on these findings, this paper describes the key pore-scale processes that control flow and trapping in a three-phase system, namely wettability order, spreading and wetting layers, and double/multiple displacement events. We show that in a porous medium containing water, oil and gas, the behaviour is controlled by wettability, which can either be water-wet, weakly oil-wet or strongly oil-wet, and by gas–oil miscibility. We provide evidence that, for the same wettability state, the three-phase pore-scale events are different under near-miscible conditions—where the gas–oil interfacial tension is ≤ 1 mN/m—compared to immiscible conditions. In a water-wet system, at immiscible conditions, water is the most-wetting phase residing in the corners of the pore space, gas is the most non-wetting phase occupying the centres, while oil is the intermediate-wet phase spreading in layers sandwiched between water and gas. This fluid configuration allows for double capillary trapping, which can result in more gas trapping than for two-phase flow. At near-miscible conditions, oil and gas appear to become neutrally wetting to each other, preventing oil from spreading in layers; instead, gas and oil compete to occupy the centre of the larger pores, while water remains connected in wetting layers in the corners. This allows for the rapid production of oil since it is no longer confined to movement in thin layers. In a weakly oil-wet system, at immiscible conditions, the wettability order is oil–water–gas, from most to least wetting, promoting capillary trapping of gas in the pore centres by oil and water during water-alternating-gas injection. This wettability order is altered under near-miscible conditions as gas becomes the intermediate-wet phase, spreading in layers between water in the centres and oil in the corners. This fluid configuration allows for a high oil recovery factor while restricting gas flow in the reservoir. Moreover, we show evidence of the predicted, but hitherto not reported, wettability order in strongly oil-wet systems at immiscible conditions, oil–gas–water, from most to least wetting. At these conditions, gas progresses through the pore space in disconnected clusters by double and multiple displacements; therefore, the injection of large amounts of water to disconnect the gas phase is unnecessary. We place the analysis in a practical context by discussing implications for carbon dioxide storage combined with enhanced oil recovery before suggesting topics for future work. [ABSTRACT FROM AUTHOR]

X-ray micro-tomography combined with a high-pressure high-temperature flow apparatus and advanced image analysis techniques were used to image and study fluid distribution, wetting states and oil recovery during low salinity waterflooding (LSW) in a complex carbonate rock at subsurface conditions. The sample, aged with crude oil, was flooded with low salinity brine with a series of increasing flow rates, eventually recovering 85% of the oil initially in place in the resolved porosity. The pore and throat occupancy analysis revealed a change in fluid distribution in the pore space for different injection rates. Low salinity brine initially invaded large pores, consistent with displacement in an oil-wet rock. However, as more brine was injected, a redistribution of fluids was observed; smaller pores and throats were invaded by brine and the displaced oil moved into larger pore elements. Furthermore, in situ contact angles and curvatures of oil–brine interfaces were measured to characterize wettability changes within the pore space and calculate capillary pressure. Contact angles, mean curvatures and capillary pressures all showed a shift from weakly oil-wet towards a mixed-wet state as more pore volumes of low salinity brine were injected into the sample. Overall, this study establishes a methodology to characterize and quantify wettability changes at the pore scale which appears to be the dominant mechanism for oil recovery by LSW. [ABSTRACT FROM AUTHOR]

We predict waterflood displacement on a pore-by-pore basis using pore network modelling. The pore structure is captured by a high-resolution image. We then use an energy balance applied to images of the displacement to assign an average contact angle, and then modify the local pore-scale contact angles in the model about this mean to match the observed displacement sequence. Two waterflooding experiments on oil-wet rocks are analysed where the displacement sequence was imaged using time-resolved synchrotron imaging. In both cases the capillary pressure in the model matches the experimentally obtained values derived from the measured interfacial curvature. We then predict relative permeability for the full saturation range. Using the optimised contact angles distributed randomly in space has little effect on the predicted capillary pressures and relative permeabilities, indicating that spatial correlation in wettability is not significant in these oil-wet samples. The calibrated model can be used to predict properties outside the range of conditions considered in the experiment. [ABSTRACT FROM AUTHOR]

We use fast synchrotron X-ray microtomography to understand three-phase flow inmixed-wet porous media to design either enhanced permeability or capillary trapping. The dynamics ofthese phenomena are of key importance in subsurface hydrology, carbon dioxide storage, oil recovery, foodand drug manufacturing, and chemical reactors. We study the dynamics of a water-gas-water injectionsequence in a mixed-wet carbonate rock. During the initial waterflooding, water displaced oil from pores ofall size, indicating a mixed-wet system with local contact angles both above and below 90◦. When gas wasinjected, gas displaced oil preferentially with negligible displacement of water. This behavior is explainedin terms of the gas pressure needed for invasion. Overall, gas behaved as the most nonwetting phase withoil as the most wetting phase; however, pores of all size were occupied by oil, water, and gas, as a signatureof mixed-wet media. Thick oil wetting layers were observed, which increased oil connectivity andfacilitated its flow during gas injection. A chase waterflooding resulted in additional oil flow, while gas wastrapped by oil and water. Furthermore, we quantified the evolution of the surface areas and both Gaussianand the total curvature, from which capillary pressure could be estimated. These quantities are related tothe Minkowski functionals which quantify the degree of connectivity and trapping. The combination ofwater and gas injection, under mixed-wet immiscible conditions, leads to both favorable oil flow andsignificant trapping of gas, which is advantageous for storage applications. [ABSTRACT FROM AUTHOR]

A quantitative in situ characterization of the impact of surface roughness on wettability in porous media is currently lacking. We use reservoir condition micrometer-resolution X-ray tomography combined with automated methods for the measurement of contact angle, interfacial curvature, and surface roughness to examine fluid/fluid and fluid/solid interfaces inside a porous material. We study oil and water in the pore space of limestone from a giant producing oilfield, acquiring millions of measurements of curvature and contact angle on three millimeter-sized samples. We identify a distinct wetting state with a broad distribution of contact angle at the submillimeter scale with a mix of water-wet and water-repellent regions. Importantly, this state allows both fluid phases to flow simultaneously over a wide range of saturation. We establish that, in media that are largely water wet, the interfacial curvature does not depend on solid surface roughness, quantified as the local deviation from a plane. However, where there has been a significant wettability alteration, rougher surfaces are associated with lower contact angles and higher interfacial curvature. The variation of both contact angle and interfacial curvature increases with the local degree of roughness. We hypothesize that this mixed wettability may also be seen in biological systems to facilitate the simultaneous flow of water and gases; furthermore, wettability-altering agents could be used in both geological systems and material science to design a mixed-wetting state with optimal process performance. [ABSTRACT FROM AUTHOR]

In the color gradient lattice Boltzmann model (CG-LBM), a fictitious-density wetting boundary condition has been widely used because of its ease of implementation. However, as we show, this may lead to inaccurate results in some cases. In this paper, a new scheme for the wetting boundary condition is proposed which can handle complicated 3D geometries. The validity of our method for static problems is demonstrated by comparing the simulated results to analytical solutions in 2D and 3D geometries with curved boundaries. Then, capillary rise simulations are performed to study dynamic problems where the three-phase contact line moves. The results are compared to experimental results in the literature (Heshmati and Piri, 2014). If a constant contact angle is assumed, the simulations agree with the analytical solution based on the Lucas–Washburn equation. However, to match the experiments, we need to implement a dynamic contact angle that varies with the flow rate. [ABSTRACT FROM AUTHOR]

Abstract: Pore-scale imaging and modelling – digital core analysis – is becoming a routine service in the oil and gas industry, and has potential applications in contaminant transport and carbon dioxide storage. This paper briefly describes the underlying technology, namely imaging of the pore space of rocks from the nanometre scale upwards, coupled with a suite of different numerical techniques for simulating single and multiphase flow and transport through these images. Three example applications are then described, illustrating the range of scientific problems that can be tackled: dispersion in different rock samples that predicts the anomalous transport behaviour characteristic of highly heterogeneous carbonates; imaging of super-critical carbon dioxide in sandstone to demonstrate the possibility of capillary trapping in geological carbon storage; and the computation of relative permeability for mixed-wet carbonates and implications for oilfield waterflood recovery. The paper concludes by discussing limitations and challenges, including finding representative samples, imaging and simulating flow and transport in pore spaces over many orders of magnitude in size, the determination of wettability, and upscaling to the field scale. We conclude that pore-scale modelling is likely to become more widely applied in the oil industry including assessment of unconventional oil and gas resources. It has the potential to transform our understanding of multiphase flow processes, facilitating more efficient oil and gas recovery, effective contaminant removal and safe carbon dioxide storage. [Copyright &y& Elsevier]

Abstract: We measure the trapped non-wetting phase saturation as a function of the initial saturation in sand packs. The application of the work is for CO2 storage in aquifers where capillary trapping is a rapid and effective mechanism to render injected CO2 immobile. The CO2 is injected into the formation followed by chase brine injection, or natural groundwater flow, which displaces and traps CO2 on the pore scale as a residual immobile phase. Current models to predict the amount of trapping are based on experiments in consolidated media, while CO2 may be stored in relatively shallow, poorly consolidated systems. We use analogue fluids at ambient conditions. The trapped saturation initially rises linearly with initial saturation to a value of approximately 0.13 for oil/water systems and 0.14 for gas/water systems. There then follows a region where the residual saturation is constant with further increases in initial saturation. This behaviour is not predicted by the traditional literature trapping models, but is physically consistent with unconsolidated media where most of the larger pores can easily be invaded at relatively low saturation and there is, overall, relatively little trapping. A good match to our experimental data was achieved with the trapping model proposed by Aissaoui. [Copyright &y& Elsevier]

Abstract: We measure the trapped non-wetting phase saturation as a function of the initial saturation in sand packs. The application of the work is for carbon dioxide (CO2) storage in aquifers where capillary trapping is a rapid and effective mechanism to render injected CO2 immobile. We used analogue fluids at ambient conditions. The trapped saturation initially rises linearly with initial saturation to a value of 0.11 for oil/water systems and 0.14 for gas/water systems. There then follows a region where the residual saturation is constant with further increases in initial saturation. [Copyright &y& Elsevier]

The development of high-resolution in situ imaging has allowed contact angles to be measured directly inside porous materials. We evaluate the use of concepts in integral geometry to determine contact angle. Specifically, we test the hypothesis that it is possible to determine an average contact angle from measurements of the Gaussian curvature of the fluid/fluid meniscus using the Gauss-Bonnet theorem. We show that it is not possible to unambiguously determine an average contact angle from the Gauss-Bonnet theorem. We instead present an approximate relationship: 2 π n (1 - cos θ) = 4 π - ∫ κ G 12 dS 12 , where n is the number of closed loops of the three-phase contact line where phases 1 and 2 contact the surface, θ is the average contact angle, while κ G 12 is the Gaussian curvature of the fluid meniscus which is integrated over its surface S 12 . We then use the results of pore-scale lattice Boltzmann simulations to assess the accuracy of this approach to determine a representative contact angle for two-phase flow in porous media. We show that in simple cases with a flat solid surface, the approximate expression works well. When applied to simulations on pore space images, the equation provides a robust estimate of contact angle, accurate to within 3 ° , when averaged over many fluid clusters, although individual values can have significant errors because of the approximations used in the calculation. [ABSTRACT FROM AUTHOR]

Based on energy balance during two-phase displacement in porous media, it has recently been shown that a thermodynamically consistent contact angle can be determined from micro-tomography images. However, the impact of viscous dissipation on the energy balance has not been fully understood. Furthermore, it is of great importance to determine the spatial distribution of wettability. We use direct numerical simulation to validate the determination of the thermodynamic contact angle both in an entire domain and on a pore-by-pore basis. Two-phase direct numerical simulations are performed on complex 3D porous media with three wettability states: uniformly water-wet, uniformly oil-wet, and non-uniform mixed-wet. Using the simulated fluid configurations, the thermodynamic contact angle is computed, then compared with the input contact angles. The impact of viscous dissipation on the energy balance is quantified; it is insignificant for water flooding in water-wet and mixed-wet media, resulting in an accurate estimation of a representative contact angle for the entire domain even if viscous effects are ignored. An increasing trend in the computed thermodynamic contact angle during water injection is shown to be a manifestation of the displacement sequence. Furthermore, the spatial distribution of wettability can be represented by the thermodynamic contact angle computed on a pore-by-pore basis. [ABSTRACT FROM AUTHOR]

[Display omitted] The 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. X-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. Development 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. [ABSTRACT FROM AUTHOR]

We define contact angles, θ , during displacement of three fluid phases in a porous medium using energy balance, extending previous work on two-phase flow. We test if this theory can be applied to quantify the three contact angles and wettability order in pore-scale images of three-phase displacement. For three phases labelled 1, 2 and 3, and solid, s , using conservation of energy ignoring viscous dissipation (Δ a 1 s cos θ 12 - Δ a 12 - ϕ κ 12 Δ S 1) σ 12 = (Δ a 3 s cos θ 23 + Δ a 23 - ϕ κ 23 Δ S 3) σ 23 + Δ a 13 σ 13 , where ϕ is the porosity, σ is the interfacial tension, a is the specific interfacial area, S is the saturation, and κ is the fluid–fluid interfacial curvature. Δ represents the change during a displacement. The third contact angle, θ 13 can be found using the Bartell-Osterhof relationship. The energy balance is also extended to an arbitrary number of phases. X-ray imaging of porous media and the fluids within them, at pore-scale resolution, allows the difference terms in the energy balance equation to be measured. This enables wettability, the contact angles, to be determined for complex displacements, to characterize the behaviour, and for input into pore-scale models. Two synchrotron imaging datasets are used to illustrate the approach, comparing the flow of oil, water and gas in a water-wet and an altered-wettability limestone rock sample. We show that in the water-wet case, as expected, water (phase 1) is the most wetting phase, oil (phase 2) is intermediate wet, while gas (phase 3) is most non-wetting with effective contact angles of θ 12 ≈ 48 ° and θ 13 ≈ 44 ° , while θ 23 = 0 since oil is always present in spreading layers. In contrast, for the altered-wettability case, oil is most wetting, gas is intermediate-wet, while water is most non-wetting with contact angles of θ 12 = 134 ° ± ~ 10 ° , θ 13 = 119 ° ± ~ 10 ° , and θ 23 = 66 ° ± ~ 10 °. [ABSTRACT FROM AUTHOR]

Conservation of energy is used to derive a thermodynamically-consistent contact angle, θ t , when fluid phase 1 displaces phase 2 in a porous medium. Assuming no change in Helmholtz free energy between two local equilibrium states we find that Δ a 1 s cos θ t = κ ϕ Δ S 1 + Δ a 12 , where a is the interfacial area per unit volume, ϕ is the porosity, S is the saturation and κ the curvature of the fluid-fluid interface. The subscript s denotes the solid, and we consider changes, Δ , in saturation and area. With the advent of high-resolution time-resolved three-dimensional X-ray imaging, all the terms in this expression can be measured directly. We analyse imaging datasets for displacement of oil by water in a water-wet and a mixed-wet sandstone. For the water-wet sample, the curvature is positive and oil bulges into the brine with almost spherical interfaces. In the mixed-wet case, larger interfacial areas are found, as the oil resides in layers. The mean curvature is close to zero, but the interface tends to bulge into brine in one direction, while brine bulges into oil in the other. We compare θ t with the values measured geometrically in situ on the pore-scale images, θ g . The thermodynamic angle θ t provides a robust and consistent characterization of wettability. For the water-wet case the calculated value of θ t gives an accurate prediction of multiphase flow properties using pore-scale modelling. [ABSTRACT FROM AUTHOR]

Wettability design is of crucial importance for the optimization of multiphase flow behaviour in gas diffusion layers (GDLs) in fuel cells. The accumulation of electrochemically-generated water in the GDLs will impact fuel cell performance. Hence, it is necessary to understand multiphase displacement to design optimal pore structures and wettability to allow the rapid flow of gases and water in GDLs over a wide saturation range. This work uses high-resolution in situ three-dimensional X-ray imaging combined with a pore network model to investigate the breakthrough capillary pressure and water saturation in GDLs manufactured with different mass fractions of polytetrafluoroethylene coating: 5, 20, 40, and 60%, making them more hydrophobic. We first demonstrate that the pore network extraction method provides representative networks for the fibrous porous media examined. Then, using a pore-network flow model we simulate water invasion into initially gas-filled fibrous media, and analyze the effect of wettability on breakthrough capillary pressure and water saturation. With an appropriate pore-scale characterization of wettability, a pore network model can match experimental results and predict displacement behaviour. • Pore network modelling is extended to study fibrous materials. • The model estimates water breakthrough pressure accurately. • The model is extended to study primary imbibition and drainage in mixed-wet media. • A representative wettability can be determined to match experiment. [ABSTRACT FROM AUTHOR]

Highlights • We obtained micro scale three-dimensional images of three-phase flow in situ at high temperature and pressure in a water-wet carbonate rock. • Pore occupancy is quantified: brine, oil and gas occupy the centre of respectively small, intermediate and large pores. • Double drainage and double imbibition are visualized in three-dimensions. • Spreading oil layers and water wetting layers are observed and their thickness allows for effective flow. • Wettability and the formation of oil layers favour trapping of gas over oil when the three phases are simultaneously present in the pore space. Abstract X-ray micro-tomography is used to image the pore-scale configurations of fluid in a rock saturated with three phases - brine, oil and gas - mimicking a subsurface reservoir, at high pressure and temperature. We determine pore occupancy during a displacement sequence that involves waterflooding, gas injection and water re-injection. In the water-wet sample considered, brine occupied the smallest pores, gas the biggest, while oil occupied pores of intermediate size and is displaced by both water and gas. Double displacement events have been observed, where gas displaces oil that displaces water or vice versa. The thickness of water and oil layers have been quantified, as have the contact angles between gas and oil, and oil and water. These results are used to explain the nature of trapping in three-phase flow, specifically how oil preferentially traps gas in the presence of water. [ABSTRACT FROM AUTHOR]

• We provided new multiphase flow measurements in a carbonate limestone with complex geometry and wettability. • We discussed its unique features related to contact angle, pore occupancy, curvature, capillary pressure and relative permeability. • The relative permeability values were corrected by considering the measured saturation profile along the sample length to correct for the so-called capillary end effect. • Greyscale based differential imaging was used and demonstrated for accurately determining the porosity and saturation without segmentation. • We demonstrated that not only wettability but also pore size distribution and microporosity have significant impact on displacement processes. Pore-scale X-ray imaging combined with a steady-state flow experiment was used to study the displacement processes during waterflooding in an altered-wettability carbonate, Ketton limestone, with more than two orders of magnitude difference in pore size between macropores and microporosity. We simultaneously characterized macroscopic and local multiphase flow parameters, including relative permeability, capillary pressure, wettability, and fluid occupancy in pores and throats. An accurate method was applied for porosity and fluid saturation measurements using greyscale based differential imaging without image segmentation. The relative permeability values were corrected by considering the measured saturation profile along the sample length to account for the so-called capillary end effect. The behaviour of relative permeability and capillary pressure was compared to other measurements in the literature to demonstrate the combined effects of wettability and pore structure. Typical oil-wet behaviour in resolvable macropores was measured from contact angle, fluid occupancy and curvature. The capillary pressure was negative while the oil relative permeability dropped quickly as oil was drained to low saturation and flowed through connected oil layers. Brine initially largely flowed through water-wet microporosity, and then filled the centre of large oil-wet pore bodies. Thus, the brine relative permeability remained exceptionally low until brine formed a connected flow path in the macropores leading to a substantial increase in relative permeability. Overall, this work demonstrates that not only wettability but also pore size distribution and microporosity have significant impact on displacement processes. [ABSTRACT FROM AUTHOR]

To better understand asphaltene deposition mechanisms and their influence on rock permeability and wettability, we have developed an in situ micro-CT imaging capability to observe asphaltene precipitation during multiphase flow at high resolution in three dimensions. Pure heptane and crude oil were simultaneously injected to induce asphaltene precipitation in the pore space of a sandstone rock sample. The heptane permeability across the sample was nine times lower after the first asphaltene precipitation, while it was reduced by a factor of ninety due to asphaltene migration and growth after subsequent brine injection. Furthermore, through quantifying the curvatures and contact angles on the images before and after asphaltene precipitation, we observed that the wettability of the porous medium changed from water-wet to mixed-wet. Overall, we demonstrate a micro-CT imaging and analysis workflow to quantify asphaltene deposition, permeability reduction and wettability change which can be used for reservoir characterisation and remediation. [ABSTRACT FROM AUTHOR]