Imperial College London

DrBrankoBijeljic

Faculty of EngineeringDepartment of Earth Science & Engineering

Principal Research Fellow
 
 
 
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Contact

 

+44 (0)20 7594 6420b.bijeljic

 
 
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Location

 

2.53Royal School of MinesSouth Kensington Campus

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Summary

 

Publications

Publication Type
Year
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171 results found

Oliveira R, Blunt MJ, Bijeljic B, 2022, Impact of physical heterogeneity and transport conditions on effective reaction rates in dissolution, Transport in Porous Media, ISSN: 0169-3913

A continuous-time random walk (CTRW) reactive transport model is used to study the impact of physical heterogeneity on the effective reaction rates in porous media in a sample of length 15 cm over timescales up to 108 s (3 years). The model has previously been validated using nuclear magnetic resonance (NMR) measurements during dissolution of a limestone. The model assumes first-order reaction. We construct three domains with increasing physical heterogeneity and study dissolution at four Péclet numbers, Pe = 0.0542, 0.542, 5.42 and 54.2. We characterize signatures of physical heterogeneity in the three porous media using velocity distributions and show how these imprint on the signatures of particle displacement, namely particle propagator distributions. In addition, we demonstrate the ability of our CTRW model to capture the impact of physical heterogeneity on the longitudinal dispersion coefficient over several orders of magnitude in space and time. Reactive transport simulations show that the effective reaction rates depend on (i) initial physical heterogeneity and (ii) transport conditions. For all heterogeneities and Pe, the late-time reaction rate exhibits a time dependence t−a with a≠0.5 that indicates the persistence of incomplete mixing. We show that the higher the initial heterogeneity, the lower the late-time reaction rate. A decrease in Pe promotes mixing by diffusion over advection, resulting in higher reaction rates. The post-dissolution propagators indicate an increase in the degree of non-Fickian transport. Overall, we establish a framework to demonstrate and quantify the impact of physical heterogeneity on transport and effective reaction rates in porous media.

Journal article

Selem AM, Agenet N, Blunt MJ, Bijeljic Bet al., 2022, Pore-scale processes in tertiary low salinity waterflooding in a carbonate rock: Micro-dispersions, water film growth, and wettability change., J Colloid Interface Sci, Vol: 628, Pages: 486-498

HYPOTHESIS: 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. EXPERIMENTS: 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. FINDINGS: 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.

Journal article

Raeini AQ, Giudici LM, Blunt MJ, Bijeljic Bet al., 2022, Generalized network modelling of two-phase flow in a water-wet and mixed-wet reservoir sandstone: Uncertainty and validation with experimental data, Advances in Water Resources, Vol: 164, Pages: 1-14, ISSN: 0309-1708

We use a generalized pore network model in combination with image-based experiments to understand the parameters that control upscaled flow properties. The study is focued on water-flooding through a reservoir sandstone under water-wet and mixed-wet conditions. A set of sensitivity studies is presented to quantify the role of wettability, pore geometry, initial and boundary conditions as well as a selection of model parameters used in the computation of fluid volumes, curvatures and flow and electrical conductivities. We quantify the uncertainty in the model predictions, which match the measured relative permeability and capillary pressure within the uncertainty of the experiments. Our results show that contact angle, initial saturation, image quality and image processing algorithm are amongst the parameters which introduce the largest variance in the predictions of upscaled flow properties for both mixed-wet and water-wet conditions.

Journal article

Zhang Y, Lin Q, Raeini AQ, Onaka Y, Iwama H, Takabayashi K, Blunt MJ, Bijeljic Bet al., 2022, Pore-scale imaging of asphaltene deposition with permeability reduction and wettability alteration, Fuel, Vol: 316, Pages: 1-9, ISSN: 0016-2361

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.

Journal article

Shojaei MJ, Bijeljic B, Zhang Y, Blunt MJet al., 2022, Minimal surfaces in porous materials: x-ray image-based measurement of the contact angle and curvature in gas diffusion layers to design optimal performance of fuel cells, ACS Applied Energy Materials, Vol: 5, Pages: 4613-4621, ISSN: 2574-0962

We inject water at a low flow rate through gas diffusion layers containing different percentages of polytetrafluoroethylene (PTFE) coating: 5, 20, 40, and 60%. We use high-resolution three-dimensional X-ray imaging to identify the arrangement of fibers, water, and air in the pore space. We also quantify the contact angle and meniscus curvature once the water has spanned the layer, flow has ceased, and water has reached a position of equilibrium. The average contact angle and water pressure at breakthrough increase with the amount of coating, although we see a wide range of contact angles with values both above and below 90°, indicating a mixed-wet state. We identify that the menisci form minimal surfaces (interfaces of zero curvature) consistent with pinned gas-water-solid contacts. Scanning electron microscopy images of the fibers show that the coated fibers have a rough surface. Between 93 and 100% of the contacts identified were found on the rough, hydrophobic, coated fibers or at the boundary between uncoated (hydrophilic) and coated (hydrophobic) regions; we hypothesize that these contacts are pinned. The one exception is the 60% PTFE layer, which shows distinctly hydrophobic properties and a negative capillary pressure (the water pressure is higher than that of air). The presence of minimal surfaces suggests that the water and gas pressures are equal, allowing water to flow readily without pressure build-up. From topological principles, the negative Gaussian curvature of the menisci implies that the fluid phases are well connected. The implication of these results is explored for the design of porous materials where the simultaneous flow of two phases occurs over a wide saturation range.

Journal article

Zhang Y, Bijeljic B, Blunt MJ, 2022, Nonlinear multiphase flow in hydrophobic porous media, Journal of Fluid Mechanics, Vol: 934, Pages: 1-10, ISSN: 0022-1120

Multiphase flow in porous materials is conventionally described by an empirical extension to Darcy's law, which assumes that the pressure gradient is proportional to the flow rate. Through a series of two-phase flow experiments, we demonstrate that even when capillary forces are dominant at the pore scale, there is a nonlinear intermittent flow regime with a power-law dependence between pressure gradient and flow rate. Energy balance is used to predict accurately the start of the intermittent regime in hydrophobic porous media. The pore-scale explanation of the behaviour based on the periodic filling of critical flow pathways is confirmed through 3D micron-resolution X-ray imaging.

Journal article

Alhosani A, Selem AM, Lin Q, Bijeljic B, Blunt MJet al., 2021, Disconnected gas transport in steady‐state three‐phase flow, Water Resources Research, Vol: 57, Pages: 1-26, ISSN: 0043-1397

We use high-resolution three-dimensional X-ray microtomography to investigate fluid displacement during steady-state three-phase flow in a cm-sized water-wet sandstone rock sample. The pressure differential across the sample is measured which enables the determination of relative permeability; capillary pressure is also estimated from the interfacial curvature. Though the measured relative permeabilities are consistent, to within experimental uncertainty, with values obtained without imaging on larger samples, we discover a unique flow dynamics. The most non-wetting phase (gas) is disconnected across the system: gas flows by periodically opening critical flow pathways in intermediate-sized pores. While this phenomenon has been observed in two-phase flow, here it is significant at low flow rates, where capillary forces dominate at the pore-scale. Gas movement proceeds in a series of double and multiple displacement events. Implications for the design of three-phase flow processes and current empirical models are discussed: the traditional conceptualization of three-phase dynamics based on analogies to two-phase flow vastly over-estimates the connectivity and flow potential of the gas phase.

Journal article

Lin Q, Bijeljic B, Raeini AQ, Rieke H, Blunt MJet al., 2021, Drainage capillary pressure distribution and fluid displacement in a heterogeneous laminated sandstone, Geophysical Research Letters, Vol: 48, Pages: 1-11, ISSN: 0094-8276

We applied three-dimensional X-ray microtomography to image a capillary drainage process (0–1,000 kPa) in a cm-scale heterogeneous laminated sandstone containing three distinct regions with different pore sizes to study the capillary pressure. We used differential imaging to distinguish solid, macropore, and five levels of subresolution pore phases associated with each region. The brine saturation distribution was computed based on average CT values. The nonwetting phase displaced the wetting phase in order of pore size and connectivity. The drainage capillary pressure in the highly heterogeneous rock was dependent on the capillary pressures in the individual regions as well as distance to the boundary between regions. The complex capillary pressure distribution has important implications for accurate water saturation estimation, gas and/or oil migration and the capillary rise of water in heterogeneous aquifers.

Journal article

Selem AM, Agenet N, Gao Y, Raeini AQ, Blunt MJ, Bijeljic Bet al., 2021, Pore-scale imaging and analysis of low salinity waterflooding in a heterogeneous carbonate rock at reservoir conditions, Scientific Reports, Vol: 11, Pages: 1-14, ISSN: 2045-2322

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.

Journal article

Shams M, Singh K, Bijeljic B, Blunt MJet al., 2021, Direct numerical simulation of pore-scale trapping events during capillary-dominated two-phase flow in porous media, Transport in Porous Media, Vol: 138, Pages: 443-458, ISSN: 0169-3913

This study focuses on direct numerical simulation of imbibition, displacement of the non-wetting phase by the wetting phase, through water-wet carbonate rocks. We simulate multiphase flow in a limestone and compare our results with high-resolution synchrotron X-ray images of displacement previously published in the literature by Singh et al. (Sci Rep 7:5192, 2017). We use the results to interpret the observed displacement events that cannot be described using conventional metrics such as pore-to-throat aspect ratio. We show that the complex geometry of porous media can dictate a curvature balance that prevents snap-off from happening in spite of favourable large aspect ratios. We also show that pinned fluid-fluid-solid contact lines can lead to snap-off of small ganglia on pore walls; we propose that this pinning is caused by sub-resolution roughness on scales of less than a micron. Our numerical results show that even in water-wet porous media, we need to allow pinned contacts in place to reproduce experimental results.

Journal article

Lin Q, Bijeljic B, Foroughi S, Berg S, Blunt MJet al., 2021, Pore-scale imaging of displacement patterns in an altered-wettability carbonate, Chemical Engineering Science, Vol: 235, Pages: 1-12, ISSN: 0009-2509

High-resolution X-ray imaging combined with a steady-state flow experiment is used to demonstrate how pore-scale displacement affects macroscopic properties in an altered-wettability microporous carbonate, where porosity and fluid saturation can be directly obtained from the grey-scale micro-CT images. The resolvable macro pores are largely oil-wet with an average thermodynamic contact angle of 120°. The pore-by-pore analysis shows locally either oil or brine almost fully occupied the macro pores, with some oil displacement in the micro-porosity. We observed a typical oil-wet behaviour consistent with the contact angle measurement. The brine tended to occupy the larger macro pores, leading to a higher brine relative permeability, lower residual oil saturation, than under water-wet conditions and in a mixed-wet sandstone. The capillary pressure was negative and seven times larger in the carbonate than the sandstone, despite having a similar average pore size. These different displacement patterns are principally determined by the difference in wettability.

Journal article

Foroughi S, Bijeljic B, Blunt MJ, 2021, Pore-by-pore modelling, validation and prediction of waterflooding in oil-wet rocks using dynamic synchrotron data, Transport in Porous Media, Vol: 138, Pages: 285-308, ISSN: 0169-3913

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.

Journal article

Alhosani A, Bijeljic B, Blunt MJ, 2021, Pore-scale imaging and analysis of wettability order, trapping and displacement in three-phase flow in porous media with various wettabilities, Transport in Porous Media, Vol: 140, Pages: 59-84, ISSN: 0169-3913

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

Journal article

Zhang Y, Bijeljic B, Gao Y, Lin Q, Blunt MJet al., 2021, Quantification of non‐linear multiphase flow in porous media, Geophysical Research Letters, Vol: 48, Pages: 1-7, ISSN: 0094-8276

We measure the pressure difference during two‐phase flow across a sandstone sample for a range of injection rates and fractional flows of water, the wetting phase, during an imbibition experiment. We quantify the onset of a transition from a linear relationship between flow rate and pressure gradient to a nonlinear power‐law dependence. We show that the transition from linear (Darcy) to nonlinear flow and the exponent in the power‐law is a function of fractional flow. We use energy balance to accurately predict the onset of intermittency for a range of fractional flows, fluid viscosities, and different rock types.

Journal article

Oliveira R, Bijeljic B, Blunt MJ, Colbourne A, Sederman AJ, Mantle MD, Gladden LFet al., 2021, A continuous time random walk approach to predict dissolution in porous media based on validation of experimental NMR data, Advances in Water Resources, Vol: 149, Pages: 1-16, ISSN: 0309-1708

We develop a reactive transport model for dissolution of porous materials using a Continuous Time Random Walk (CTRW) formulation with first-order kinetics. Our model is validated with a dataset for a Ketton carbonate rock sample undergoing dissolution on injection of an acid, monitored using Nuclear Magnetic Resonance (NMR). The experimental data includes the 3D porosity distribution at the beginning and end of the experiment, 1D porosity profiles along the direction of flow during dissolution, as well as the molecular fluid displacement probability distributions (propagators). With the calibration of only a single parameter, we successfully predict the porosity changes and the propagators as a signature of flow heterogeneity evolution in the dissolution experiment.We also demonstrate that heterogeneity in the flow field leads to an effective reaction rate, limited by transport of reactants, that is almost three orders of magnitude lower than measured under batch reaction conditions. The effective reaction rate predicted by the model is in good agreement with the experimentally measured rate. Furthermore, as dissolution proceeds, the formation of channels in the rock focused the flow in a few fast-flowing regions. The predicted dissolution patterns are similar to those observed experimentally. This study establishes a workflow to calibrate and validate the CTRW reactive transport model with NMR experiments.

Journal article

Alhosani A, Lin Q, Scanziani A, Andrews E, Zhang K, Bijeljic B, Blunt MJet al., 2021, Pore-scale characterization of carbon dioxide storage at immiscible and near-miscible conditions in altered-wettability reservoir rocks, International Journal of Greenhouse Gas Control, Vol: 105, Pages: 1-15, ISSN: 1750-5836

Carbon dioxide storage combined with enhanced oil recovery (CCS-EOR) is an important approach for reducing greenhouse gas emissions. We use pore-scale imaging to help understand CO2 storage and oil recovery during CCS-EOR at immiscible and near-miscible CO2 injection conditions. We study in situ immiscible CO2 flooding in an oil-wet reservoir rock at elevated temperature and pressure using X-ray micro-tomography. We observe the predicted, but hitherto unreported, three-phase wettability order in strongly oil-wet rocks, where water occupies the largest pores, oil the smallest, while CO2 occupies pores of intermediate size. We investigate the pore occupancy, existence of CO2 layers, recovery and CO2 trapping in the oil-wet rock at immiscible conditions and compare to the results obtained on the same rock type under slightly more weakly oil-wet near-miscible conditions, with the same wettability order. CO2 spreads in connected layers at near-miscible conditions, while it exists as disconnected ganglia in medium-sized pores at immiscible conditions. Hence, capillary trapping of CO2 by oil occurs at immiscible but not at near-miscible conditions. Moreover, capillary trapping of CO2 by water is not possible in both cases since CO2 is more wetting to the rock than water. The oil recovery by CO2 injection alone is reduced at immiscible conditions compared to near-miscible conditions, where low gas-oil capillary pressure improves microscopic displacement efficiency. Based on these results, to maximize the amount of oil recovered and CO2 stored at immiscible conditions, a water-alternating-gas injection strategy is suggested, while a strategy of continuous CO2 injection is recommended at near-miscible conditions.

Journal article

Blunt MJ, Alhosani A, Lin Q, Scanziani A, Bijeljic Bet al., 2021, Determination of contact angles for three-phase flow in porous media using an energy balance, Journal of Colloid and Interface Science, Vol: 582, Pages: 283-290, ISSN: 0021-9797

HYPOTHESIS: 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. THEORY: For three phases labelled 1, 2 and 3, and solid, s, using conservation of energy ignoring viscous dissipation (Δa1scosθ12-Δa12-ϕκ12ΔS1)σ12=(Δa3scosθ23+Δa23-ϕκ23ΔS3)σ23+Δa13σ13, 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, θ13 can be found using the Bartell-Osterhof relationship. The energy balance is also extended to an arbitrary number of phases. FINDINGS: 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 θ12≈48° and θ13≈44°, while θ23=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 θ12=134°±~10°,θ13=119°&p

Journal article

Selem AM, Agenet N, Blunt MJ, Bijeljic Bet al., 2021, Pore-scale imaging of tertiary low salinity waterflooding in a heterogeneous carbonate rock at reservoir conditions

We investigated pore-scale oil displacement and rock wettability in tertiary low salinity waterflooding (LSW) in a heterogeneous carbonate sample using high-resolution three-dimensional imaging. This enabled the underlying mechanisms of the low salinity effect (LSE) to be observed and quantified in terms of changes in wettability and pore-scale fluid configuration, while also measuring the overall effect on recovery. The results were compared to the behavior under high salinity waterflooding (HSW). To achieve the wetting state found in oil reservoirs, an Estaillades limestone core sample was aged at 11 MPa and 80°C for threeweeks. The moderately oil-wet sample was then injected with high salinity brine (HSB) at a range of increasing flow rates, namely at 1, 2,4, 11, 22 and 42 µL/min with 10 pore volumes injected at each rate.Subsequently, low salinity brine (LSB) was injected following the same procedure. X-ray micro-computed tomography (micro-CT) was usedto visualize the fluid configuration in the pore space.A total of eight micro-CT images, with a resolution of 2.3 µm/voxel, wereacquired after both low salinity and high salinity floods.These high-resolution images were used to monitor fluid configuration in the porespace and obtain fluid saturations and occupancy maps. Wettabilitywascharacterized by measurements of in situ contactanglesand curvatures. The results show that the pore-scale mechanisms of improved recovery in LSW are consistent with the development of water micro-dropletswithin the oil and the expansion of thin water films between the oil and rock surface. Before waterflooding and during HSW, the measured contact angles were constant and above 110°, while the meancurvature and the capillary pressure values remained negative, suggesting that the HSB did not change the wettability state of the rock. However, with LSW the capillary pressure increased towards positive values as the wettability shifted towards a mixed-wet state. The flu

Conference paper

Blunt M, Kearney L, Alhosani A, Lin Q, Bijeljic Bet al., 2021, Wettability characterization from pore-scale images using topology and energy balance with implications for recovery and storage

We present two methods to measure contact angles inside porous media using high-resolution images. The direct determination of contact angle at the three-phase contact line is often ambiguous due to uncertainties with image segmentation. Instead, we propose two alternative approaches that provide an averaged assessment of wettability. The first uses fundamental principles in topology to relate the contact angle to the integral of the Gaussian curvature over the fluid-fluid meniscus. The advantage of this approach is that it replaces the uncertain determination of an angle at a point with a more accurate determination of an integral over a surface. However, in mixed-wet porous media, many interfaces are pinned with a hinging contact angle. For predictive pore-scale models, we need to determine the contact angle at which displacement occurs when the interfaces move. To address this problem we apply an energy balance, ignoring viscous dissipation, to estimate the contact angle from the meniscus curvature and changes in interfacial areas and saturation. We apply these methods to characterize wettability on pore-scale images of two- and three-phase flow. We also discuss the implications of the results for recovery and storage applications.

Conference paper

Gao Y, Raeini AQ, Blunt MJ, Bijeljic Bet al., 2021, Dynamic fluid configurations in steady-state two-phase flow in Bentheimer sandstone, Physical Review E, Vol: 103, ISSN: 2470-0045

Fast synchrotron tomography is used to study the impact of capillary number, Ca, on fluid configurations in steady-state two-phase flow in porous media. Brine and n-decane were co-injected at fixed fractional flow, fw=0.5, in a cylindrical Bentheimer sandstone sample for a range of capillary numbers 2.1×10−7≤Ca≤4.2×10−5, while monitoring the pressure differential. As we have demonstrated in Gao et al. [Phys. Rev. Fluids 5, 013801 (2020)], dependent on Ca, different flow regimes have been identified: at low Ca only fixed flow pathways exist, while after a certain threshold dynamic effects are observed resulting in intermittent fluctuations in fluid distribution which alter fluid connectivity. Additionally, the flow paths, for each capillary number, were imaged multiple times to quantify the less frequent changes in fluid occupancy, happening over timescales longer than the duration of our scans (40 s). In this paper we demonstrate how dynamic connectivity results from the interaction between oil ganglia populations. At low Ca connected pathways of ganglia are fixed with time-independent small, medium, and large ganglia populations. However, with an increase in Ca we see fluctuations in the size and numbers of the larger ganglia. With the onset of intermittency, fluctuations occur mainly in pores and throats of intermediate size. When Ca is further increased, we see rapid changes in occupancy in pores of all size. By combining observations on pressure fluctuations and flow regimes at various capillary numbers, we summarize a phase diagram over a range of capillary numbers for the wetting and nonwetting phases, Caw and Canw, respectively, to quantify the degree of intermittent flow. These different regimes are controlled by a competition between viscous forces on the flowing fluids and the capillary forces acting in the complex pore space. Furthermore, we plot the phase diagrams of the transition from Darcy flow to intermittent flow over a

Journal article

Selem A, Agenet N, Gao Y, Lin Q, Blunt MJ, Bijeljic Bet al., 2021, PORE-SCALE IMAGING OF CONTROLLED-SALINITY WATERFLOODING IN A HETEROGENEOUS CARBONATE ROCK AT RESERVOIR CONDITIONS, Pages: 2272-2276

Controlled salinity water-flooding (CSW) is a promising enhanced oil recovery technique, yet the pore-scale mechanisms that control the process remain poorly understood especially in carbonate rocks. The aim of this experimental study is, therefore, to gain novel insights into CSW and characterize oil, water and the pore space in carbonates. X-ray imaging combined with a high-pressure high-temperature flow apparatus was used to image and study in situ CSW in a complex carbonate rock. To establish the conditions found in oil reservoirs, the Estaillades limestone core sample (5.9 mm in diameter and 10 mm in length) was aged for three weeks at 11 MPa and 80°C. This weakly oil-wet sample was then flooded by injecting low salinity brine at a range of increasing flow rates. Tomographic images were acquired at 2.9-micron spatial resolution after each flow rate. A total of 60 pore volumes of low salinity brine were injected recovering 85% of the oil initially in place in macro-pores. Contact angles and brine-oil curvatures were obtained to characterize wettability changes within the rock pore space. Our analysis shows that wettability alteration towards a mixed wet system caused by low salinity brine was the main mechanism for increased oil recovery.

Conference paper

Lin Q, Akai T, Blunt MJ, Bijeljic B, Iwama H, Takabayashi K, Onaka Y, Yonebayashi Het al., 2021, Pore-scale imaging of asphaltene-induced pore clogging in carbonate rocks, Fuel, Vol: 283, ISSN: 0016-2361

We propose an experimental methodology to visualize asphaltene precipitation in the pore space of rocks and assess the reduction in permeability. We perform core flooding experiments integrated with X-ray microtomography (micro-CT). The simultaneous injection of pure heptane and crude oil containing asphaltene induces the precipitation of asphaltene in the pore space. The degree of precipitation is controlled by the measurement of differential pressure across the sample. After precipitation, doped heptane is injected to replace the fluid to enhance the contrast between precipitated asphaltene and doped heptane. The micro-CT images are segmented into three phases: void, precipitated asphaltene, and rock. In the experiment, we observed that the precipitated asphaltene which occupied 39.1% of the pore volume caused a 29-fold reduction in permeability. Furthermore, we analyze the spatial distribution of precipitated asphaltene which showed that the asphaltene tended to clog the larger pores. We also computed the flow field numerically on the images and obtained good agreement between simulated and measured permeability. The distribution of local velocity showed that after precipitation the flow was confined to narrow channels in the pore space. This method can be applied to any type of porous system with precipitation.

Journal article

Alhosani A, Scanziani A, Lin Q, Selem A, Pan Z, Blunt MJ, Bijeljic Bet al., 2020, Three-phase flow displacement dynamics and Haines jumps in a hydrophobic porous medium, Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol: 476, ISSN: 1364-5021

We use synchrotron X-ray micro-tomography to investigate the displacement dynamics during three-phase—oil, water and gas—flow in a hydrophobic porous medium. We observe a distinct gas invasion pattern, where gas progresses through the pore space in the form of disconnected clusters mediated by double and multiple displacement events. Gas advances in a process we name three-phase Haines jumps, during which gas re-arranges its configuration in the pore space, retracting from some regions to enable the rapid filling of multiple pores. The gas retraction leads to a permanent disconnection of gas ganglia, which do not reconnect as gas injection proceeds. We observe, in situ, the direct displacement of oil and water by gas as well as gas–oil–water double displacement. The use of local in situ measurements and an energy balance approach to determine fluid–fluid contact angles alongside the quantification of capillary pressures and pore occupancy indicate that the wettability order is oil–gas–water from most to least wetting. Furthermore, quantifying the evolution of Minkowski functionals implied well-connected oil and water, while the gas connectivity decreased as gas was broken up into discrete clusters during injection. This work can be used to design CO2 storage, improved oil recovery and microfluidic devices.

Journal article

Oliveira TDS, Blunt M, Bijeljic B, Serafini de Oliveira T, Blunt M, Bijeljic Bet al., 2020, Multispecies reactive transport in a microporous rock: impact of flow heterogeneity and reversibility of reaction, Water Resources Research, Vol: 56, ISSN: 0043-1397

We study the impact of pore space heterogeneity on mixing and reaction in porous media. We simulate the parallel injection of two streams of reactants at different pH in a three-dimensional microporous consolidated rock whose pore space was resolved by differential micro-CT imaging. As an exemplar of a heterogeneous medium, we consider the pore structure obtained from a Portland carbonate sample. We use direct numerical simulation to study the coupled impact of flow heterogeneity, characterized by a wide distribution of velocities, and chemical reversibility on multispecies reaction. The flow field is found from the Darcy-Brinkman equation while the advection-diffusion equation describes transport, which is coupled to a general multispecies geochemical solver for homogeneous reactions; precipitation and dissolution are ignored.We observe a highly non-uniform spatial distribution of concentration and rates of formation and consumption. For advection-dominated transport, the heterogeneous flow field leads to significant transverse mixing in macropores at early times, followed by a slower mixing driven by diffusion between macro- and micropore regions. The effective rates of formation and consumption are species-dependent and distinct in macro- and microporosity: while some species reach an asymptotic rate in well-mixed regions, others still show a transient non-monotonic behaviour as a consequence of incomplete mixing. Our findings have important implications for the understanding of time- and space-dependent reaction rate behaviour: the coupled impact of pore space heterogeneity and reversible reactions need to be taken into account as key determinants to describe multispecies reactive transport.

Journal article

Gao Y, Raeini AQ, Selem AM, Bondino I, Blunt MJ, Bijeljic Bet al., 2020, Pore-scale imaging with measurement of relative permeability and capillary pressure on the same reservoir sandstone sample under water-wet and mixed-wet conditions, Advances in Water Resources, Vol: 146, Pages: 1-18, ISSN: 0309-1708

Using micro-CT imaging and differential pressure measurements, we design a comparative study in which we simultaneously measure relative permeability and capillary pressure on the same reservoir sandstone sample under water-wet and mixed-wet conditions during steady-state waterflooding experiments. This allows us to isolate the impact of wettability on a pore-by-pore basis and its effect on the macroscopic parameters, capillary pressure and relative permeability, while keeping the pore-space geometry unchanged.First, oil and brine were injected through a water-wet reservoir sandstone sample at a fixed total flow rate, but in a sequence of increasing brine fractional flows with micro-CT scans of the fluid phases taken in each step. Then the sample was brought back to initial water saturation and the surface wettability of the sample was altered after prolonged contact with crude oil and the same measurement procedure was repeated on the altered-wettability sample which we call mixed-wet.Geometric contact angles were measured, which discriminated the water-wet and mixed-wet cases with average values of 75° and 89° respectively. Additionally, an energy balance was used to determine the effective contact angles for displacement which indicated that a higher advancing contact angle of 116° was needed to displace oil in the mixed-wet case. For the water-wet experiment the filling sequence was pore-size dependent, with a strong correlation between pore size and oil occupancy. However, in the mixed-wet experiment the principal determinant of the filling sequence was the wettability rather than the pore size, and there was no correlation between pore size and the residual oil occupancy.The oil-water interfacial area had a larger maximum in the mixed-wet case which was supported by the observation of sheet or saddle-like menisci shapes present throughout the sample volume that impede the flow. These shapes were quantified by much larger negative Gaussian curvature

Journal article

Akai T, Lin Q, Bijeljic B, Blunt MJet al., 2020, Using energy balance to determine pore-scale wettability, Journal of Colloid and Interface Science, Vol: 576, Pages: 486-495, ISSN: 0021-9797

HypothesisBased 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.SimulationsTwo-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.FindingsThe 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.

Journal article

Blunt MJ, Akai T, Bijeljic B, 2020, Evaluation of methods using topology and integral geometry to assess wettability, JOURNAL OF COLLOID AND INTERFACE SCIENCE, Vol: 576, Pages: 99-108, ISSN: 0021-9797

Journal article

Scanziani A, Alhosani A, Lin Q, Spurin C, Garfi G, Blunt MJ, Bijeljic Bet al., 2020, In situ characterization of three‐phase flow in mixed‐wet porous media using synchrotron imaging, Water Resources Research, Vol: 56, ISSN: 0043-1397

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.

Journal article

Alhosani A, Scanziani A, Lin Q, Foroughi S, Alhammadi AM, Blunt MJ, Bijeljic Bet al., 2020, Dynamics of water injection in an oil-wet reservoir rock at subsurface conditions: Invasion patterns and pore-filling events, Physical Review E, Vol: 102, Pages: 023110 – 1-023110 – 15, ISSN: 2470-0045

We use fast synchrotron x-ray microtomography to investigate the pore-scale dynamics of water injection in an oil-wet carbonate reservoir rock at subsurface conditions. We measure, in situ, the geometric contact angles to confirm the oil-wet nature of the rock and define the displacement contact angles using an energy-balance-based approach. We observe that the displacement of oil by water is a drainagelike process, where water advances as a connected front displacing oil in the center of the pores, confining the oil to wetting layers. The displacement is an invasion percolation process, where throats, the restrictions between pores, fill in order of size, with the largest available throats filled first. In our heterogeneous carbonate rock, the displacement is predominantly size controlled; wettability has a smaller effect, due to the wide range of pore and throat sizes, as well as largely oil-wet surfaces. Wettability only has an impact early in the displacement, where the less oil-wet pores fill by water first. We observe drainage associated pore-filling dynamics including Haines jumps and snap-off events. Haines jumps occur on single- and/or multiple-pore levels accompanied by the rearrangement of water in the pore space to allow the rapid filling. Snap-off events are observed both locally and distally and the capillary pressure of the trapped water ganglia is shown to reach a new capillary equilibrium state. We measure the curvature of the oil-water interface. We find that the total curvature, the sum of the curvatures in orthogonal directions, is negative, giving a negative capillary pressure, consistent with oil-wet conditions, where displacement occurs as the water pressure exceeds that of the oil. However, the product of the principal curvatures, the Gaussian curvature, is generally negative, meaning that water bulges into oil in one direction, while oil bulges into water in the other. A negative Gaussian curvature provides a topological quantification of th

Journal article

Scanziani A, Lin Q, Alhosani A, Blunt MJ, Bijeljic B, Scanziani A, Lin Q, Alhosani A, Blunt M, Bijeljic Bet al., 2020, Dynamics of fluid displacement in mixed-wet porous media, Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol: 476, Pages: 1-16, ISSN: 1364-5021

We identify a distinct two-phase flow invasion pattern in a mixed-wet porous medium. Time-resolved high-resolution synchrotron X-ray imaging is used to study the invasion of water through a small rock sample filled with oil, characterized by a wide non-uniform distribution of local contact angles both above and below 90°. The water advances in a connected front, but throats are not invaded in decreasing order of size, as predicted by invasion percolation theory for uniformly hydrophobic systems. Instead, we observe pinning of the three-phase contact between the fluids and the solid, manifested as contact angle hysteresis, which prevents snap-off and interface retraction. In the absence of viscous dissipation, we use an energy balance to find an effective, thermodynamic, contact angle for displacement and show that this angle increases during the displacement. Displacement occurs when the local contact angles overcome the advancing contact angles at a pinned interface: it is wettability which controls the filling sequence. The product of the principal interfacial curvatures, the Gaussian curvature, is negative, implying well-connected phases which is consistent with pinning at the contact line while providing a topological explanation for the high displacement efficiencies in mixed-wet media.

Journal article

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