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Observations over a range of scales show that lowering the salinity of injected water can alter the wetting state of a rock, making it more water-wet. However, there remains a poor understanding of...

Hypothesis: The wetting behaviour is a key property of a porous medium that controls hydraulic conductivity in multiphase flow. While many porous materials, such as hydrocarbon reservoir rocks, are initially wetted by the aqueous phase, surface active components within the non-wetting phase can alter the wetting state of the solid. Close to the saturation endpoints wetting phase fluid films of nanometre thickness impact the wetting alteration process. The properties of these films depend on the chemical characteristics of the system. Here we demonstrate that surface texture can be equally important and introduce a novel workflow to characterize the wetting state of a porous medium. Experiments: We investigated the formation of fluid films along a rock surface imaged with atomic force microscopy using zeta-potential measurements and a computational model for drainage. The results were compared to spontaneous imbibition test to link sub-pore-scale and core-scale wetting characteristics of the rock. Findings: The results show a dependency between surface coverage by oil, which controls the wetting alteration, and the macroscopic wetting response. The surface-area coverage is dependent on the capillary pressure applied during primary drainage. Close to the saturation endpoint, where the change in saturation was minor, the oil-solid contact changed more than 80%. (C) 2019 The Authors. Published by Elsevier Inc.

Understanding the interaction between competing fluids in the pore space of rocks is key for predicting subsurface flow and trapping, such as with CO2 in a saline aquifer. These processes occur over a large span of timescales (from seconds to thousands of years), and length scales (from microns to kilometres). Understanding the link between these temporal and spatial scales will enable us to interpolate between observations made at different resolutions. In this work we explore the temporal scales present during macroscopically steady-state multiphase flow in a porous rock using differential pressure measurements. We observe a cascade of timescales in the pressure differential i.e. a continuous range of frequencies, with lower frequencies having greater amplitudes. We demonstrate a scaling of the spectral density with frequency of S ∼ 1/f^2, or red noise, to describe the dynamics. This scaling is independent of the flow rate of the fluids or the fraction of the flow taken by water. This red, or Brownian, noise indicates a stochastic process where pressure fluctuations are seen throughout the pore space, resulting in intermittent filling of pores over a wide range of time-scales, from seconds to minutes in these experiments. This observation will aid future modelling of subsurface flow as it suggests self-organised critically of the system with no characteristic time or length scale.

Hypothesis: The macroscopic movement of subsurface fluids involved in CO2 storage, groundwater, and petroleum engineering applications is controlled by interfacial forces in the pores of rocks. Recent advances in modelling these systems has arisen from approaches simulating flow through a digital representation of the complex pore structure. However, further progress is limited by difficulties in characterising the spatial distribution of the wetting state within the pore structure. In this work, we show how observations of the fluid coverage of mineral surfaces within the pores of rocks can be used as the basis for a quantitative 3D characterisation of heterogeneous wetting states throughout rock pore structures. Experiments: We demonstrate the approach with water–oil fluid pairs on rocks with distinct lithologies (sandstone and carbonate) and wetting states (hydrophilic, intermediate wetting, and heterogeneously wetting). Findings: Fluid surface coverage the within rock pores is a robust signal of the wetting state across varying rock types and wetting states. The wetting state can be quantified and the resulting 3D maps can be used as a deterministic input to pore scale models. These may be applied to multiphase flow problems in porous media ranging from soil science to fuel cells.

We use fast synchrotron X‐ray microtomography to understand three‐phase flow in mixed‐wet porous media to design either enhanced permeability or capillary trapping. The dynamics of these phenomena are of key importance in subsurface hydrology, carbon dioxide storage, oil recovery, food and drug manufacturing, and chemical reactors. We study the dynamics of a water‐gas‐water injection sequence in a mixed‐wet carbonate rock. During the initial waterflooding, water displaced oil from pores of all size, indicating a mixed‐wet system with local contact angles both above and below 90°. When gas was injected, gas displaced oil preferentially with negligible displacement of water. This behavior is explained in terms of the gas pressure needed for invasion. Overall, gas behaved as the most nonwetting phase with oil as the most wetting phase; however, pores of all size were occupied by oil, water, and gas, as a signature of mixed‐wet media. Thick oil wetting layers were observed, which increased oil connectivity and facilitated its flow during gas injection. A chase waterflooding resulted in additional oil flow, while gas was trapped by oil and water. Furthermore, we quantified the evolution of the surface areas and both Gaussian and the total curvature, from which capillary pressure could be estimated. These quantities are related to the Minkowski functionals which quantify the degree of connectivity and trapping. The combination of water and gas injection, under mixed‐wet immiscible conditions, leads to both favorable oil flow and significant trapping of gas, which is advantageous for storage applications.

The wetting state is an important control on flow in subsurface multi fluid phase systems, e.g., carbon storage and oil production. Advances in X-ray imaging allow us to characterise the wetting state using imagery of fluid arrangement within the pores of rocks. We derived a model from equilibrium thermodynamics relating fluid coverage of rock surfaces to wettability and fluid saturation. The model reproduces the behaviour measured in a water-wet, nearly all-quartz, Bentheimer sandstone imaged during steady-state imbibition. A shift in fluid surface coverage is observed when the rock is altered to a new wetting state with crude oil. In two multi-mineralogical (Berea) samples, one water-wet and the other altered with crude oil, the analysis of fluid surface coverage after imbibition revealed mineral specific wetting preferences only in the altered system. Clays and calcite preferentially alter to an oil wet state, leading to mixed wettability in the rock.

Many subsurface fluid flows, including the storage of CO2 underground or the production of oil, are transient processes incorporating multiple fluid phases. The fluids are not in equilibrium meaning macroscopic properties such as fluid saturation and pressure vary in space and time. However, these flows are traditionally modeled with equilibrium (or steady-state) flow properties, under the assumption that the pore-scale fluid dynamics are equivalent. In this work, we used fast synchrotron X-ray tomography with 1 s time resolution to image the pore-scale fluid dynamics as the macroscopic flow transitioned to steady state. For nitrogen or decane, and brine injected simultaneously into a porous rock, we observed distinct pore-scale fluid dynamics during transient flow. Transient flow was found to be characterized by intermittent fluid occupancy, whereby flow pathways through the pore space were constantly rearranging. The intermittent fluid occupancy was largest and most frequent when a fluid initially invaded the rock. But as the fluids established an equilibrium the dynamics decreased to either static interfaces between the fluids or small-scale intermittent flow pathways, depending on the capillary number and viscosity ratio. If the fluids were perturbed after an equilibrium was established, by changing the flow rate, the transition to a new equilibrium was quicker than the initial transition. Our observations suggest that transient flows require separate modeling parameters. The time scales required to achieve equilibrium suggest that several meters of an invading plume front will have flow properties controlled by transient pore-scale fluid dynamics.

The wetting state is an important control on flow in subsurface multi fluid phase systems, e.g., carbon storage and oil production. Advances in X-ray imaging allow us to characterise the wetting state using imagery of fluid arrangement within the pores of rocks. We derived a model from equilibrium thermodynamics relating fluid coverage of rock surfaces to wettability and fluid saturation. The model reproduces the behaviour measured in a water-wet, nearly all-quartz, Bentheimer sandstone imaged during steady-state imbibition. A shift in fluid surface coverage is observed when the rock is altered to a new wetting state with crude oil. In two multi-mineralogical (Berea) samples, one water-wet and the other altered with crude oil, the analysis of fluid surface coverage after imbibition revealed mineral specific wetting preferences only in the altered system. Clays and calcite preferentially alter to an oil wet state, leading to mixed wettability in the rock.

X-ray microcomputed tomography (X-ray μ-CT) is a rapidly advancing technology that has been successfully employed to study flow phenomena in porous media. It offers an alternative approach to core scale experiments for the estimation of traditional petrophysical properties such as porosity and single-phase flow permeability. It can also be used to investigate properties that control multiphase flow such as rock wettability or mineral topology. In most applications, analyses are performed on segmented images obtained employing a specific processing pipeline on the greyscale images. The workflow leading to a segmented image is not straightforward or unique and, for most of the properties of interest, a ground truth is not available. For this reason, it is crucial to understand how image processing choices control properties estimation. In this work, we assess the sensitivity of porosity, permeability, specific surface area, in situ contact angle measurements, fluid–fluid interfacial curvature measurements and mineral composition to processing choices. We compare the results obtained upon the employment of two processing pipelines: non-local means filtering followed by watershed segmentation; segmentation by a manually trained random forest classifier. Single-phase flow permeability, in situ contact angle measurements and mineral-to-pore total surface area are the most sensitive properties, as a result of the sensitivity to processing of the phase boundary identification task. Porosity, interfacial fluid–fluid curvature and specific mineral descriptors are robust to processing. The sensitivity of the property estimates increases with the complexity of its definition and its relationship to boundary shape.

Intermittent fluid flow has recently been identified as an important transport mode for processes involving subsurface multiphase fluids such as CO 2 storage and natural gas production. However, due to experimental limitations, it has not been possible to identify why intermittency occurs at subsurface conditions and what the implications are for upscaled flow properties such as relative permeability. We address these questions with observations of nitrogen and brine flowing at steady-state through a carbonate rock. We overcome previous imaging limitations with high-speed (1s resolution), synchrotron-based X-ray micro-computed tomography combined with pressure measurements recorded while controlling fluid flux. We observe that intermittent fluid transport allows the non-wetting phase to flow through a more ramified network of pores, which would not be possible with connected pathway flow alone for the same flow rate. The volume of fluid intermittently fluctuating increases with capillary number, with the corresponding expansion of the flow network minimising the role of inertial forces in controlling flow even as the flow rate increases. Intermittent pathway flow sits energetically between laminar and turbulent through connected pathways. While a more ramified flow network favours lowered relative permeability, intermittency is more dissipative than laminar flow through connected pathways, and the relative permeability remains unchanged for low capillary numbers where the pore geometry controls the location of intermittency. However, as the capillary number increases further, the role of pore structure in controlling intermittency decreases which corresponds to an increase in relative permeability. These observations can serve as the basis of a model for the causal links between intermittent fluid flow, fluid distribution throughout the pore space, and the upscaled manifestation in relative permeability.