Experimental investigation of carbon dioxide trapping due to capillary retention in saline aquifers

Capillary trapping is a physical mechanism by which carbon dioxide (CO₂) is naturally immobilized in the pore spaces of aquifer rocks during geologic carbon sequestration operations, and thus a key aspect of estimating geologic storage potential. Here, we studied capillary trapping of supercritical carbon dioxide (scCO₂), and the effect of initial scCO₂ saturation and flow rate on the storage/trapping potential of Berea sandstone. We performed two‐phase, scCO₂‐brine displacements in two samples, each subject to four sequential drainage–imbibition core‐flooding cycles to quantify end‐point saturations of scCO₂ with the aid of micro‐ and macro‐computed tomography imaging. From these experiments, we found that between 51% and 75% of the initial CO₂ injected can be left behind after the brine injection. We also observed that the initial scCO₂ saturation influenced the residual scCO₂ saturation to a greater extent than the rate of brine injection under the experimental conditions examined. In spite of differences in the experimental conditions tested, as well as those reported in the literature, initial and residual saturations were found to follow a consistent relationship.     

Gas breakthrough experiments on fine-grained sedimentary rocks

The capillary sealing efficiency of fine‐grained sedimentary rocks has been investigated by gas breakthrough experiments on fully water saturated claystones and siltstones (Boom Clay from Belgium, Opalinus Clay from Switzerland and Tertiary mudstone from offshore Norway) of different lithological compositions. Sand contents of the samples were consistently below 12%, major clay minerals were illite and smectite. Porosities determined by mercury injection lay between 10 and 30% while specific surface areas determined by nitrogen adsorption (BET method) ranged from 20 to 48 m² g ^{? 1}. Total organic carbon contents were below 2%. Prior to the gas breakthrough experiments the absolute (single phase) permeability (k_abs) of the samples was determined by steady state flow tests with water or NaCl brine. The k_abs values ranged between 3 and 550 nDarcy (3 × 10^?21 and 5.5 × 10^?19 m²). The maximum effective permeability to the gas‐phase (k_eff) measured after gas breakthrough on initially water‐saturated samples extended from 0.01 nDarcy (1 × 10^?23 m²) up to 1100 nDarcy (1.1 × 10^?18 m²). The residual differential pressures after re‐imbibition of the water phase, referred to as the ‘minimum capillary displacement pressures’ (P_d), ranged from 0.06 to 6.7 MPa. During the re‐imbibition process the effective permeability to the gas phase decreases with decreasing differential pressure. The recorded permeability/pressure data were used to derive the pore size distribution (mostly between 8 and 60 nm) and the transport porosity of the conducting pore system (10^‐5–10^‐2%). Correlations could be established between (i) absolute permeability coefficients and the maximum effective permeability coefficients and (ii) effective or absolute permeability coefficients and capillary sealing efficiency. No correlation was found between the capillary displacement pressures determined from gas breakthrough experiments and those derived theoretically by mercury injection.     

Capillary Active Interior Insulation Systems for Wall Retrofitting: A More Nuanced Story

To thermally upgrade exterior masonry walls, interior insulation is often the only possible retrofitting technique, especially when dealing with historic buildings. Unfortunately, it is also the riskiest post-insulation technique, as frost damage, interstitial condensation, and other damage patterns might be induced. To diminish those risks, nowadays so-called capillary active interior insulation systems are often promoted. These systems aim a minimal reduction of the inward drying potential, while interstitial condensation is buffered.

Currently, several capillary active systems are on sale. These different types have, however, widely varying properties. In this article, a closer look at the hygrothermal properties and the working principle of a number of “capillary active” interior insulation systems is made. The spread in capillary absorption coefficients and the vapor diffusion resistances of the different systems is discussed and their influence is illustrated. Based on all this, a more nuanced view on capillary active insulation systems is pursued.

Abbreviations: AC: aerated concrete; CaSi: calcium silicate; GM: glue mortar; GB: gypsum board; HAMFEM: Heat Air and Moisture Finite Element Method; MW: mineral wool; PE: polyethylene; PIR: polyisocyanurate; PUR: polyurethane; VIP: vacuum insulation panel; WFB: wood fiber board; XPS: extruded polystyrene; sd_dry: dry vapor diffusion resistance factor; µ_dry: dry vapor diffusion resistance     

In situ decarboxylation of acetic and formic acids in aqueous inclusions as a possible way to produce excess CH4

Accurate reconstruction of diagenetic P‐T conditions in petroleum reservoirs from fluid inclusion data relies on valid measurements of methane concentration in aqueous inclusions. Techniques have been developed (Raman spectrometry) to provide sufficiently accurate data, assuming measured methane concentration has not been modified after aqueous inclusion entrapment. This study investigates the likelihood that organic acids derived from petroleum fluids and dissolved in formation water might suffer decarboxylation upon postentrapment heating within the fluid inclusion chamber, thereby generating excess CH₄ in the inclusions. Four different experiments were conducted in fused silica capillary capsules (FSCCs), mimicking fluid inclusions. The capsules were loaded with acetic (CH₃COOH) or formic (HCOOH) acid solution and were heated to 250°C for short durations (<72 h) in closed‐system conditions, with or without applying a fixed P_H2. Reaction products were characterized by Raman and FT‐IR spectrometry. Results indicate that decarboxylation reactions did take place, at variable degrees of progress, and that measurable excess CH₄ was produced in one experiment using acetic acid. This suggests that methane may be produced from dissolved organic acids in natural aqueous inclusions in specific situations, possibly inducing errors in the thermodynamic interpretation.     

Faults and fault properties in hydrocarbon flow models

The petroleum industry uses subsurface flow models for two principal purposes: to model the flow of hydrocarbons into traps over geological time, and to simulate the production of hydrocarbon from reservoirs over periods of decades or less. Faults, which are three-dimensional volumes, are approximated in both modelling applications as planar membranes onto which predictions of the most important fault-related flow properties are mapped. Faults in porous clastic reservoirs are generally baffles or barriers to flow and the relevant flow properties are therefore very different to those which are important in conductive fracture flow systems. A critical review and discussion is offered on the work-flows used to predict and model capillary threshold pressure for exploration fault seal analysis and fault transmissibility multipliers for production simulation, and of the data from which the predictions derive. New flow simulation models confirm that failure of intra-reservoir sealing faults can occur during a reservoir depressurization via a water-drive mechanism, but contrary to anecdotal reports, published examples of production-induced seal failure are elusive. Ignoring the three-dimensional structure of fault zones can sometimes have a significant influence on production-related flow, and a series of models illustrating flow associated with relay zones are discussed.     

Changes in sub‐water table fluid flow at the end of the Proterozoic and its implications for gas pulsars and MVT lead–zinc deposits

A fundamental change in the nature of sub‐water table fluid flow occurred at roughly the Proterozoic–Phanerozoic boundary when organic matter began to be buried in sufficient quantities that nonaqueous fluids could occupy a significant fraction of the pore space. This allowed the formation of remarkably durable capillary seals that could trap gas in large portions (hundreds of kilometers) of a basin for hundreds of millions of years. Gas loss from these gas zones can be highly dynamic, especially during gas generation. Under the right circumstances, hundreds of cubic kilometers of gas can be rapidly discharged into adjacent permeable aquifers. In Pennsylvanian/Permian time, the Arkoma Basin may have repeatedly discharged such volumes of gas into the very permeable Cambrian sandstone and karstic carbonate aquifers of the mid‐continent of the United States. This could have displaced brines rapidly enough to form the Mississippi Valley‐type (MVT) lead–zinc deposits of this age that are associated with the Arkoma Basin, heating them only briefly as required by maturity indicators. Sea level rise accompanying the melting of Permian continental glaciers may have triggered the gas expulsion events. This radically new mechanism for the formation of MVT deposits is just one example of the nonlinear dynamics of gas accumulations that are possible since Late Proterozoic time.     

Experimental study of the effect of variation in in‐situ stress on capillary residual trapping during CO2 geo‐sequestration in sandstone reservoirs

During a geo‐sequestration process, CO₂ injection causes an increase in reservoir pore pressure, which in turn decreases the reservoir net effective stress. Changes in effective stress can change all the reservoir and cap‐rock properties including residual saturations. This article presents the results of an experimental work carried out to understand the potential change in the volumes of residually trapped CO₂, while the porous medium tested underwent change in the net effective stress under in‐situ reservoir conditions of pore pressure and temperature. The experimental results obtained show that an initial 1725 psi (11.9 MPa) decrease in the net effective pressure caused 1.4% reduction in the volumes of residually trapped CO₂, while another 1500 psi (10.3 MPa) reduction caused a further 3.2% drop in the residual saturation of CO₂.     

Soluble Salts Amplify the Effect of Small Heterogeneities in the Structure of Porous Building Materials During Drying

Salt crystallization is a major cause of degradation in old buildings. One of the issues that stills need clarification is regarding the influence of the salts on the capillary absorption and subsequent drying of porous building materials. This article presents an experimental study that included capillary absorption and evaporative drying tests on two types of material (lime mortar and ceramic brick) using pure water or saturated solutions of six salts (sodium chloride, sodium sulfate, sodium nitrate, sodium carbonate, potassium nitrate, or potassium carbonate). The results of capillary absorption agree only roughly with the linear relationship, predicted by theory, between sorptivity and the square root of the ratio between viscosity η and surface tension σ of the solution (σ/η)^1/2. This poor agreement is probably due to material heterogeneity. The drying dynamics was regular and showed little dispersion between specimens, but only for the uncontaminated materials. Indeed, the drying dynamics of the salt contaminated materials was often irregular or diverged among similar specimens, and the same happened with their salt decay patterns. The main conclusion is that soluble salts can amplify the effects on drying of the small structural heterogeneities that porous building materials normally depict.     

Quantifying secondary migration efficiencies

Exploration success relies on properly risking the hydrocarbon system relevant for each prospect. Accurate risking of secondary migration efficiencies has been difficult due to lack of simple procedures that relate rock properties such as permeability and entry pressures to migration velocities, oil stringer heights and saturations. In order to achieve improved estimates of charge probabilities, equations for the secondary migration process are formulated based upon the Darcy flow and buoyancy conditions. An analytical solution of the formulated equations is shown, making it possible to construct charts for efficiently assessing the column height of secondary migration hydrocarbon stringers. The average oil (hydrocarbon) saturation of the migrating stringer can be computed, making it easy to compute the permeability related, secondary migration losses. Inputs to the chart are hydrocarbon flow‐rates and flow‐path width, hydrocarbon viscosity and density, carrier bed dip, permeability and entry pressures. Outputs are stringer heights, hydrocarbon saturation, relative permeability, migration velocities and migration losses. A procedure for including the new equations into existing basin scale fluid flow simulators is outlined and a Java applet for calculating the properties is described. The Java applet is useful for sensitivity studies, and can also be used to test results from basin simulators with the new migration efficiency equations. The analytical solution suggests that many published methods for calculating hydrocarbon migration in fluid flow simulators will over‐estimate hydrocarbon saturations and therefore losses. Calculated migration velocities will also be too low.     

Gas breakthrough experiments on pelitic rocks: comparative study with N2, CO2 and CH4

The capillary‐sealing efficiency of intermediate‐ to low‐permeable sedimentary rocks has been investigated by N₂, CO₂ and CH₄ breakthrough experiments on initially fully water‐saturated rocks of different lithological compositions. Differential gas pressures up to 20 MPa were imposed across samples of 10–20 mm thickness, and the decline of the differential pressures was monitored over time. Absolute (single‐phase) permeability coefficients (k_abs), determined by steady‐state fluid flow tests, ranged between 10^?22 and 10^?15 m². Maximum effective permeabilities to the gas phase k_eff(max), measured after gas breakthrough at maximum gas saturation, extended from 10^?26 to 10^?18 m². Because of re‐imbibition of water into the interconnected gas‐conducting pore system, the effective permeability to the gas phase decreases with decreasing differential (capillary) pressure. At the end of the breakthrough experiments, a residual pressure difference persists, indicating the shut‐off of the gas‐conducting pore system. These pressures, referred to as the ‘minimum capillary displacement pressures’ (P_d), ranged from 0.1 up to 6.7 MPa. Correlations were established between (i) absolute and effective permeability coefficients and (ii) effective or absolute permeability and capillary displacement pressure. Results indicate systematic differences in gas breakthrough behaviour of N₂, CO₂ and CH₄, reflecting differences in wettability and interfacial tension. Additionally, a simple dynamic model for gas leakage through a capillary seal is presented, taking into account the variation of effective permeability as a function of buoyancy pressure exerted by a gas column underneath the seal.