Dynamic reservoir-condition microtomography of reactive transport in complex carbonates: effect of initial pore structure and initial brine pH

We study the impact of brine acidity and initial pore structure on the dynamics of fluid/solid reaction at high Péclet numbers and low Damköhler numbers. A laboratory μ-CT scanner was used to image the dissolution of Ketton, Estaillades, and Portland limestones in the presence of CO2-acidified brine at reservoir conditions (10 MPa and 50°C) at two injected acid strengths for a period of 4 hours. Each sample was scanned between 6 and 10 times at ∼4 μm resolution and multiple effluent samples were extracted. The images were used as inputs into flow simulations, and analysed for dynamic changes in porosity, permeability, and reaction rate. Additionally, the effluent samples were used to verify the image-measured porosity changes. We find that initial brine acidity and pore structure determine the type of dissolution. Dissolution is either uniform where the porosity increases evenly both spatially and temporally, or occurs as channelling where the porosity increase is concentrated in preferential flow paths. Ketton, which has a relatively homogeneous pore structure, dissolved uniformly at pH = 3.6 but showed more channelized flow at pH = 3.1. In Estaillades and Portland, increasingly complex carbonates, channelized flow was observed at both acidities with the channel forming faster at lower pH. It was found that the effluent pH, which is higher than that injected, is a reasonably good indicator of effective reaction rate during uniform dissolution, but a poor indicator during channelling. The overall effective reaction rate was up to 18 times lower than the batch reaction rate measured on a flat surface at the effluent pH, with the lowest reaction rates in the samples with the most channelized flow, confirming that transport limitations are the dominant mechanism in determining reaction dynamics at the fluid/solid boundary

The impact of porous media heterogeneity on non-Darcy flow behaviour from pore-scale simulation

The effect of pore-scale heterogeneity on non-Darcy flow behaviour is investigated by means of direct flow simulations on 3-D images of a beadpack, Bentheimer sandstone and Estaillades carbonate. The critical Reynolds number indicating the cessation of the creeping Darcy flow regime in Estaillades carbonate is two orders of magnitude smaller than in Bentheimer sandstone, and is three orders of magnitude smaller than in the beadpack. It is inferred from the examination of flow field features that the emergence of steady eddies in pore space of Estaillades at elevated fluid velocities accounts for the early transition away from the Darcy flow regime. The non-Darcy coefficient β, the onset of non-Darcy flow, and the Darcy permeability for all samples are obtained and compared to available experimental data demonstrating the predictive capability of our approach. X-ray imaging along with direct pore-scale simulation of flow provides a viable alternative to experiments and empirical correlations for predicting non-Darcy flow parameters such as the β factor, and the onset of non-Darcy flow

Dynamic pore-scale reservoir-condition imaging of reaction in carbonates using synchrotron fast tomography

Synchrotron fast tomography was used to dynamically image dissolution of limestone in the presence of CO2-saturated brine at reservoir conditions. 100 scans were taken at a 6.1 µm resolution over a period of 2 hours. Underground storage permanence is a major concern for carbon capture and storage. Pumping CO2 into carbonate reservoirs has the potential to dissolve geologic seals and allow CO2 to escape. However, the dissolution processes at reservoir conditions are poorly understood. Thus, time-resolved experiments are needed to observe and predict the nature and rate of dissolution at the pore scale. Synchrotron fast tomography is a method of taking high-resolution time-resolved images of complex pore structures much more quickly than traditional µ-CT . The Diamond Lightsource Pink Beam was used to dynamically image dissolution of limestone in the presence of CO2-saturated brine at reservoir conditions. 100 scans were taken at a 6.1 µm resolution over a period of 2 hours. The images were segmented and the porosity and permeability were measured using image analysis and network extraction. Porosity increased uniformly along the length of the sample; however, the rate of increase of both porosity and permeability slowed at later times

Pore-scale dynamics and the multiphase Darcy law

Synchrotron x-ray microtomography combined with sensitive pressure differential measurements were used to study flow during steady-state injection of equal volume fractions of two immiscible fluids of similar viscosity through a 57-mm-long porous sandstone sample for a wide range of flow rates. We found three flow regimes. (1) At low capillary numbers, Ca, representing the balance of viscous to capillary forces, the pressure gradient, ∇ P , across the sample was stable and proportional to the flow rate (total Darcy flux) q t (and hence capillary number), confirming the traditional conceptual picture of fixed multiphase flow pathways in porous media. (2) Beyond Ca ∗ ≈ 10 − 6 , pressure fluctuations were observed, while retaining a linear dependence between flow rate and pressure gradient for the same fractional flow. (3) Above a critical value Ca > Ca i ≈ 10 − 5 we observed a power-law dependence with ∇ P ∼ q a t with a ≈ 0.6 associated with rapid fluctuations of the pressure differential of a magnitude equal to the capillary pressure. At the pore scale a transient or intermittent occupancy of portions of the pore space was captured, where locally flow paths were opened to increase the conductivity of the phases. We quantify the amount of this intermittent flow and identify the onset of rapid pore-space rearrangements as the point when the Darcy law becomes nonlinear. We suggest an empirical form of the multiphase Darcy law applicable for all flow rates, consistent with the experimental results

Quantification of sub-resolution porosity in carbonate rocks by applying high-salinity contrast brine using X-ray microtomography differential imaging

Characterisation of the pore space in carbonate reservoirs and aquifers is of utmost importance in a number of applications such as enhanced oil recovery, geological carbon storage and contaminant transport. We present a new experimental methodology that uses high-salinity contrast brine and differential imaging acquired by X-ray tomography to non-invasively obtain three-dimensional spatially resolved information on porosity and connectivity of two rock samples, Portland and Estaillades limestones, including sub-resolution micro-porosity. We demonstrate that by injecting 30 wt% KI brine solution, a sufficiently high phase contrast can be achieved allowing accurate three-phase segmentation based on differential imaging. This results in spatially resolved maps of the solid grain phase, sub-resolution micro-pores within the grains, and macro-pores. The total porosity values from the three-phase segmentation for two carbonate rock samples are shown to be in good agreement with Helium porosity measurements. Furthermore, our flow-based method allows for an accurate estimate of pore connectivity and a distribution of porosity within the sub-resolution pores

Evaluation of methods using topology and integral geometry to assess wettability.

HYPOTHESIS: 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. THEORY AND SIMULATION: 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: 2πn(1-cosθ)=4π-∫κG12dS12, 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 κG12 is the Gaussian curvature of the fluid meniscus which is integrated over its surface S12. 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. FINDINGS: 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

Reservoir condition imaging of reactive transport in heterogeneous carbonates using fast synchrotron tomography - effect of initial pore structure and flow conditions

AbstractWe investigate the impact of initial pore structure and velocity field heterogeneity on the dynamics of fluid/solid reaction at high Péclet numbers (fast flow) and low Damköhler number (relatively slow reaction rates). The Diamond Lightsource Pink Beam was used to image dissolution of Estaillades and Portland limestones in the presence of CO2-saturated brine at reservoir conditions (10MPa and 50°C representing ~1km aquifer depth) at two flow rates for a period of 2h. Each sample was scanned between 51 and 94 times at 4.76-μm resolution and the dynamic changes in porosity, permeability, and reaction rate were examined using image analysis and flow modelling.We find that the porosity can either increase uniformly through time along the length of the samples, or may exhibit a spatially and temporally varying increase that is attributed to channel formation, a process that is distinct from wormholing, depending on initial pore structure and flow conditions. The dissolution regime was structure-dependent: Estaillades with a higher porosity showed more uniform dissolution, while the lower porosity Portland experienced channel formation. The effective reaction rates were up to two orders of magnitude lower than those measured on a flat substrate with no transport limitations, indicating that the transport of reactant and product is severely hampered away from fast flow channels