One of the critical factors that control the efficiency of CO 2 geological storage process in aquifers and hydrocarbon reservoirs is the capillary-sealing potential of the caprock. This potential can be expressed in terms of the maximum reservoir overpressure that the brine-saturated caprock can sustain, i.e. of the CO 2 capillary entry pressure. It is controlled by the brine/CO 2 interfacial tension, the water-wettability of caprock minerals, and the pore size distribution within the caprock.By means of contact angle measurements, experimental evidence was obtained showing that the water-wettability of mica and quartz is altered in the presence of CO 2 under pressures typical of geological storage conditions. The alteration is more pronounced in the case of mica. Both minerals are representative of shaly caprocks and are strongly water-wet in the presence of hydrocarbons.A careful analysis of the available literature data on breakthrough pressure measurements in caprock samples confirms the existence of a wettability alteration by dense CO 2 , both in shaly and in evaporitic caprocks. The consequences of this effect on the maximum CO 2 storage pressure and on CO 2 storage capacity in the underground reservoir are discussed. For hydrocarbon reservoirs that were initially close to capillary leakage, the maximum allowable CO 2 storage pressure is only a fraction of the initial reservoir pressure.
Directed assembly of asymmetric ternary block copolymer-homopolymer blends using symmetric block copolymer into checkerboard trimming chemical patternThe phase behavior of ternary blends of an A-B random copolymer with two homopolymers (A and B) is investigated within the Flory-Huggins lattice theory. We restrict consideration to the formation of (isotropic) liquid phases. For compositionally symmetric systems in which the two homopolymers have equal molecular weights, two different topologies are found for the phase diagrams according to the length of the copolymer relative to the homopolymers. Namely, upon lowering the temperature, a three-liquid-phase region emerges either continuously via a tricritical point if the copolymer is long enough, or discontinuously otherwise. This change in phase behavior, an entropy of mixing effect, occurs when the copolymer length is a fraction 2/5 of the homopolymer molecular weight. The properties of the (symmetric) tricritical points are discussed, as well as the phase behavior of systems in which the copolymer is not symmetrical in composition and/or the two homopolymers differ in size. This Flory-Huggins approach should be valid for blends containing random copolymers, but also, at high enough temperatures, for blends that contain block copolymers, the temperature range of validity being broader for smaller block copolymers. The critical behavior of systems containing block copolymers is described by the simple Flory-Huggins theory over a range delineated by isotropic Lifshitz points. These Lifshitz points are located within the random phase approximation.
A series of viscosimetric and small-angle neutron scattering experiments on asphaltenes diluted in mixed toluene/heptane solvents has been conducted, with the purpose of characterizing the size, molecular weight, and internal structure of asphaltene aggregates as a function of solvent conditions. With increasing flocculant (i.e., heptane) content in the solvent, the intrinsic viscosities of asphaltene aggregates first decreased, went through a minimum for heptane fractions ≈ 10−20%, and then increased at the approach of flocculation. These variations paralleled those of the volume of aggregate occupied per unit mass of asphaltene, a behavior reminiscent of the Flory−Fox relationship for polymers in a solvent. This volume, proportional to the cubed radius of gyration of the aggregates divided by their molecular weight, was determined from the neutron scattering data. For increasing heptane fractions in the solvent, the molecular weight of the aggregates increased with their radius of gyration according to a power law, the exponent being in the range of 2. This exponent also characterized the self-similar internal structure of the asphaltene aggregates. With due care to the possible systematic effects of the strong polydispersity of these aggregates, these results are discussed in light of recent models of colloidal aggregation.
The various modes of acid gas storage in aquifers, namely structural, residual, and local capillary trapping, are effective only if the rock remains water‐wet. This paper reports an evaluation, by means of the captive‐bubble method, of the water‐wet character in presence of dense acid gases (CO2, H2S) of typical rock‐forming minerals such as mica, quartz, calcite, and of a carbonate‐rich rock sampled from the caprock of a CO2 storage reservoir in the South‐West of France. The method, which is improved from that previously implemented with similar systems by Chiquet et al. (Geofluids 2007; 7: 112), allows the advancing and receding contact angles, as well as the adhesion behavior of the acid gas on the mineral substrate, to be evaluated over a large range of temperatures (up to 140°C), pressures (up to 150 bar), and brine salinities (up to NaCl saturation) representative of various geological storage conditions. The water‐receding (or gas‐advancing) angle that controls structural and local capillary trapping is observed to be not significantly altered in the presence of dense CO2 or H2S. In contrast, some alteration of the water‐advancing (or gas‐receding) angle involved in residual trapping is observed, along with acid gas adhesion, particularly on mica. A spectacular wettability reversal is even observed with mica and liquid H2S. These results complement other recent observations on similar systems and present analogies with the wetting behavior of crude oil/brine/mineral systems, which has been thoroughly studied over the past decades. An insight is given into the interfacial forces that govern wettability in acid gas‐bearing aquifers, and the consequences for acid gas geological storage are discussed along with open questions for future work.
The structure of asphaltene solutions in toluene was studied by small-angle neutron scattering (SANS) as a function of temperature and concentration. Temperature alters solvent quality, flocculation being expected at low temperature. SANS measurements were carried out at four different temperatures (from 73 down to 8 °C) for solute (asphaltene) volume fractions Φ ranging from =0.3 to ∼10%. Asphaltenes were found to form nanometric aggregates, whose average masses (Mw) and radii of gyration (RGZ) increased as temperature decreased. These parameters hardly varied with concentration in the dilute regime Φ e 3-4%, in which no evidence of dissociation was found. At higher Φ, apparent values of the same parameters (Mw and RGZ) decreased as repulsive interactions or aggregate interpenetration reduced the normalized intensity, I/Φ, a phenomenon reminiscent of the semidilute regime of polymers and fractal aggregates. At the two lowest temperatures studied, 8 and 20 °C, a strong scattering at low q signaled flocculation, as some of the asphaltenes formed dense domains of micronic size. This phenomenon occurred throughout the studied concentration range and entailed some limited hysteresis for time scales of the order of a few hours.
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