Continuum-scale convective mixing in geological CO2 sequestration in anisotropic and heterogeneous saline aquifers

Deep saline aquifers are important geological formations for CO₂ sequestration. It has been known that dissolution of CO₂ increases brine density, which results in downward density-driven convection and consequently greatly enhances CO₂ sequestration. In this study, a continuum-scale lattice Boltzmann model is used to investigate convective mixing of CO₂ in saline aquifers. It is found that increasing permeability in either the vertical or horizontal direction accelerates the development of convective mixing. In a heterogeneous aquifer, increasing heterogeneity hampers the onset of convective mixing, because the heterogeneous permeability field results in a large portion of low-velocity region which reduces the instability of the system. The critical time for the onset of instability depends mainly on the coefficient of variation (COV) of the permeability field, and is insensitive to the correlation length. This implies that within the scale of critical time, mass transport is dominated by diffusion, and thus depends mainly on fine-scale heterogeneity controlled by COV. We derived an empirical formula for estimating the critical time, which leads to good estimates for all combinations of COV and correlation length. Fingering, channeling, and dispersion are the three mechanisms for mass transport. In dispersion, dissolved mass is approximately proportional to the square root of time, while in fingering and channeling it is approximately proportional to time. Mass transport by channeling depends significantly on permeability structure, while by fingering it is controlled by gravitational instability. It is also found that larger volumes of CO₂ can be stored in heterogeneous aquifers because of higher mass dissolution rates.     

Convective stability analysis of the long-term storage of carbon dioxide in deep saline aquifers

Deep saline aquifers are one of the most suitable geologic formations for carbon sequestration. The linear and global stability analysis of the time-dependent density-driven convection in deep saline aquifers is presented for long-term storage of carbon dioxide (CO₂). The convective mixing that can greatly accelerate the CO₂ dissolution into saline aquifers arises because the density of brine increases upon the dissolution of CO₂ and such a density difference may induce instability. The effects of anisotropic permeability on the stability criteria, such as the critical time for the appearance of convective phenomena and the critical wavelength of the most unstable perturbation, are investigated with linear and global stability analysis. The linear stability analysis provides a sufficient condition for instability while the global stability analysis yields a sufficient condition for stability. The results obtained from these two approaches are not exactly the same but show a consistent trend, both indicating that the anisotropic system becomes more unstable when either the vertical or horizontal permeability increases.     

Dynamics of convective dissolution from a migrating current of carbon dioxide

During geologic storage of carbon dioxide (CO₂), trapping of the buoyant CO₂ after injection is essential in order to minimize the risk of leakage into shallower formations through a fracture or abandoned well. Models for the subsurface behavior of the CO₂ are useful for the design, implementation, and long-term monitoring of injection sites, but traditional reservoir-simulation tools are currently unable to resolve the impact of small-scale trapping processes on fluid flow at the scale of a geologic basin. Here, we study the impact of solubility trapping from convective dissolution on the up-dip migration of a buoyant gravity current in a sloping aquifer. To do so, we conduct high-resolution numerical simulations of the gravity current that forms from a pair of miscible analogue fluids. Our simulations fully resolve the dense, sinking fingers that drive the convective dissolution process. We analyze the dynamics of the dissolution flux along the moving CO₂–brine interface, including its decay as dissolved buoyant fluid accumulates beneath the buoyant current. We show that the dynamics of the dissolution flux and the macroscopic features of the migrating current can be captured with an upscaled sharp-interface model.     

Energy spectra associated with long's model for steady finite-amplitude flow over orography

Abstract

The process of wave steepening in Long's model of steady, two-dimensional stably stratified flow over orography is examined. Under conditions of the long-wave approximation, and constant values of the background static stability and basic flow, Long's equation is cast into the form of a nonlinear advection equation. Spectral properties of this latter equation, which could be useful for the interpretation of data analyses under mountain wave conditions, are presented. The principal features, that apply at the onset of convective instability (density constant with height), are:

i) a power spectrum for available potential energy that exhibits a minus eight-thirds decay, in terms of the vertical wavenumber k _z ^-;

ii) a rate of energy transfer across the spectrum that is inversely proportional to the wavenumber for large k _z ^-;

iii) an equipartition between the kinetic energy of the horizontal motion and the available potential energy, under the longwave approximation, although all the disturbance energy is kinetic at the point where convective instability is initiated. It is also shown that features i) and ii) apply to more general conditions that are appropriate to Long's model, not just the long-wave approximation. Application to fully turbulent flow or to conditions at the onset of shearing instability are not considered to be warranted, since the development only applies to conditions at the onset of convective instability.     

Distribution of the surface partial pressure of CO2 in the southern Yellow Sea and its controls

Surface partial pressure of CO₂ (pCO₂), dissolved inorganic carbon (DIC), temperature, salinity and chlorophyll a (Chl a) at grid stations were measured in the southern Yellow Sea (SYS; 32–37°N to 120–125°E) during four cruises conducted in March 2005 (winter), April 2006 (spring), May 2005 (late spring), and July 2001 (summer). Factors influencing pCO₂ spatial and seasonal variations are explored.Surface seawater pCO₂ during winter was oversaturated with respect to the atmosphere in the entire study area (380–606 μatm), primarily due to the complete mixing of the water column in winter which brought CO₂-enriched bottom water to the surface. However, during spring, surface pCO₂ in the central SYS was undersaturated relative to the atmosphere with a low range between 274 and 408 μatm. The net CO₂ sink in the central SYS was mainly due to the consumption of CO₂ by the strong phytoplankton activity and to the weak water stratification, whereas surface pCO₂ in the nearshore area was oversaturated for the atmosphere owing to vertical mixing and terrestrial inputs. During summer, surface pCO₂ varied between 125 and 599 μatm over the entire sampling area. In the Changjiang (Yangtze River) Diluted Water (CDW) area, surface pCO₂ was undersaturated because of the nutrient inputs via the Changjiang, triggering strong phytoplankton activity, whereas surface pCO₂ was oversaturated in other areas. We conclude that the nearshore area behaves as a source of atmospheric CO₂ during the entire investigated periods owing to vertical mixing and terrestrial inputs as well as upwelling, whereas the central region generally shifts from a source of CO₂ in March to a sink in the remaining time of the investigation.     

Mechanisms of along-channel sediment transport in the North Passage of the Yangtze Estuary and their response to large-scale interventions

The effects of large-scale interventions in the North Passage of the Yangtze Estuary (the Deep Waterway Project, DWP) on the along-channel flow structure, suspended sediment distribution and its transport along the main channel of this passage are investigated. The focus is explaining the changes in net sediment transport in terms of physical mechanisms. For this, data of flow and suspended sediment concentration (SSC), which were collected simultaneously at several locations and at different depths along the main channel of the North Passage prior to and after the engineering works, were harmonically analyzed to assess the relative importance of the transport components related to residual (time-mean) flow and various tidal pumping mechanisms. Expressions for main residual flow components were derived using theoretical principles. The SSC revealed that the estuarine turbidity maximum (ETM) was intensified due to the interventions, especially in wet seasons, and an upstream shift and extension of the ETM zone occurred. The amplitude of the M ₂ tidal current considerably increased, and the residual flow structure was significantly altered by engineering works. Prior to the DWP, the residual flow structure was that of a gravitational circulation in both seasons, while after the DWP, there was seaward flow throughout the channel during the wet season. The analysis of net sediment transport reveals that during wet seasons and prior to the DWP, the sediment trapping was due to asymmetric tidal mixing, gravitational circulation, tidal rectification, and M ₂ tidal pumping, while after the DWP, the trapping was primarily due to seaward transport caused by Stokes return flow and fresh water discharge and landward transport due to M ₂ tidal pumping and asymmetric tidal mixing. During dry seasons, prior to the DWP, trapping of sediment at the bottom relied on landward transports due to Stokes transport, M ₄ tidal pumping, asymmetric tidal mixing, and gravitational circulation, while after the DWP the sediment trapping was caused by M ₂ tidal pumping, Stokes transport, asymmetric tidal mixing, tidal rectification, and gravitational circulation.     

Interfacial tension measurements and wettability evaluation for geological CO2 storage

Interfacial interactions, namely interfacial tension, wettability, capillarity and interfacial mass transfer are known to govern fluid distribution and behavior in porous media. Therefore the interfacial interactions between CO₂, brine and oil and/or gas reservoirs have a significant influence on the effectiveness of any CO₂ storage operations. However, data and knowledge of interfacial properties in storage conditions are scarce. This issue becomes particularly true in the case of deep saline aquifers where limited, economically driven, data collection and archiving are available. In this paper, we present a complete set of brine–CO₂ interfacial tension data at pressure, temperature and salinity conditions, representative of a CO₂ storage operation. A semi-empirical correlation is proposed to calculate the interfacial tension from the experimental data. Wettability is studied at pore scale, using glass micromodels in order to track fluids distribution as a function of the thermodynamic properties and wettability conditions for water–CO₂ systems. With this approach, we show that, in strongly hydrophilic porous media, the CO₂ does not wet the solid surface whereas; if the porous media has less hydrophilic properties the CO₂ significantly wets the surface.     

The effect of heterogeneity on the character of density-driven natural convection of CO2 overlying a brine layer

The efficiency of mixing in density-driven natural-convection is largely governed by the aquifer permeability, which is heterogeneous in practice. The character (fingering, stable mixing or channeling) of flow-driven mixing processes depends primarily on the permeability heterogeneity character of the aquifer, i.e., on its degree of permeability variance (Dykstra-Parsons coefficient) and the correlation length. Here we follow the ideas of Waggoner et al. (1992) [13] to identify different flow regimes of a density-driven natural convection flow by numerical simulation. Heterogeneous fields are generated with the spectral method of Shinozuka and Jan (1972) [13], because the method allows the use of power-law variograms. In this paper, we extended the classification of Waggoner et al. (1992) [13] for the natural convection phenomenon, which can be used as a tool in selecting optimal fields with maximum transfer rates of CO₂ into water. We observe from our simulations that the rate of mass transfer of CO₂ into water is higher for heterogeneous media.     

Hot springs mediate spatial exchange of heat and mass in the enclosed sediment domain: A stability perspective

In many natural environments, such as in underwater hot springs and hydrothermal vents, thermal gradients are accompanied with changes in the concentration of chemical compounds transported to the seawater, causing the so-called double-diffusive, mixed convection. To study the physical scenarios in such systems, a vertical channel filled with a porous medium saturated with saline water is considered. The motion in the sediment-filled channel is induced by two buoyancy forces and an external pressure gradient, similar to the situation in a vent with an upward flow direction. The fluid flow has been modeled by an extended Darcy model, and the flow instability mechanisms have been studied numerically. The linear stability analysis is performed considering a wide range of Darcy number (Da = 10⁻⁵ -10⁻⁸). The instability boundary curve showed three distinct dynamic regimes: (i) Rayleigh-Taylor (R-T), (ii) log-log non-linear variation, and (iii) log-log linear variation. The domain of different regimes were sensitive to external pressure gradient as well as permeability. Similar to cross-diffusive natural convection in pure viscous fluids, a linear relationship between logarithmic absolute values of critical thermal Rayleigh number (∣Ra_T∣) and solute Rayleigh number (Ra_C) is found in the third regime. Based on the permeability, for any solute Rayleigh number (Ra_C), there existed a minimum value of Reynolds number (Re), below which R-T type of instability appeared. Above this minimum value, the instability was due to two buoyancy forces, known as buoyant instability. Simulations of secondary flow via energy analysis demonstrated the development of complex dynamics at the critical state in all three regimes characterized by transition of multi to uni-cellular structures and vice verse.     

Influence of capillary-pressure models on CO2 solubility trapping

The typical shape of a capillary-pressure curve is either convex (e.g., Brooks–Corey model) or S-shaped (e.g., van Genuchten model). It is not universally agreed which model reflects natural rocks better. The difference between the two models lies in the representation of the capillary entry pressure. This difference does not lead to significantly different simulation results for modeling CO₂ sequestration in aquifers without considering CO₂ dissolution. However, we observe that the van-Genuchten-type capillary-pressure model accelerates CO₂ solubility trapping significantly compared with the Brooks–Corey-type model. We also show that the simulation results are very sensitive to the slope of the van-Genuchten-type curve around the entry-pressure region. For the representative examples we study, the differences can be so large as to have complete dissolution of the CO₂ plume versus persistence of over 50% of the plume over a 5000-year period.The cause of such sensitivity to the capillary-pressure model is studied. Particularly, we focus on how the entry pressure is represented in each model. We examine the mass-transfer processes under gravity-capillary equilibrium, molecular diffusion, convective mixing, and in the presence of small-scale heterogeneities. Laboratory measurement of capillary-pressure curves and some important implementation issues of capillary-pressure models in numerical simulators are also discussed. Most CO₂ sequestration simulations in the literature employ one of the two capillary-pressure models. It is important to recognize that these two representations lead to very different predictions of long-term CO₂ sequestration.     

Interfacial tension between CO2 and brine (NaCl + CaCl2) at elevated pressures and temperatures: The additive effect of different salts

An extensive laboratory study was conducted to measure the interfacial tension (IFT) between CO₂ and brine consisting in equal molal concentrations of NaCl and CaCl₂. The experiments were repeated at various pressures, temperatures and salinities that are representative of conditions prevailing during CO₂ storage in deep saline aquifers. The dependence of CO₂/brine IFT on pressure and temperature is similar to that previously reported for the systems: CO₂/NaCl solution and CO₂/CaCl₂ solution. CO₂/brine IFT increases linearly with water salinity and the magnitude of this increase was found equal to the sum of the individual CO₂/NaCl solution and CO₂/CaCl₂ solution IFT increments, indicating a strong additive effect on IFT when the brine is composed of various salts.     

Effects of CO2 on benthic biota: An in situ benthic chamber experiment in Storfjorden (Norway)

Carbon capture and storage (CCS) methods, either sub-seabed or in ocean depths, introduces risk of CO₂ leakage and subsequent interaction with the ecosystem. It is therefore important to obtain information on possible effects of CO₂. In situ CO₂ exposure experiments were carried out twice for 10 days during 2005 using a Benthic Chamber system at 400 m depth in Storfjorden, Norway. pCO₂ in the water above the sediment in the chambers was controlled at approximately 500, 5000 and 20,000 μatm, respectively. This article describes the experiment and the results from measured the biological responses within the chamber sediments. The results show effects of elevated CO₂ concentrations on biological processes such as increased nanobenthos density. Methane production and sulphate reduction was enhanced in the approximately 5000 μatm chamber.     

Instability of flows near the onset of convection in a rotating layer with stress-free horizontal boundaries

We investigate instability of convective flows of simple structure (rolls, standing and travelling waves) in a rotating layer with stress-free horizontal boundaries near the onset of convection. We show that the flows are always unstable to perturbations, which are linear combinations of large-scale modes and short-scale modes, whose wave numbers are close to those of the perturbed flows. Depending on asymptotic relations of small parameters α (the difference between the wave number of perturbed flows and the critical wave number for the onset of convection) and ε (ε² being the overcriticality and the perturbed flow amplitude being O(ε)), either small-angle or Eckhaus instability is prevailing. In the case of small-angle instability for rolls the largest growth rate scales as ε^8/5, in agreement with results of Cox and Matthews (Cox, S.M. and Matthews, P.C., Instability of rotating convection. J. Fluid. Mech., 2000, 403, 153–172) obtained for rolls with k = k _c . For waves, the largest growth rate is of the order ε^4/3. In the case of Eckhaus instability the growth rate is of the order of α².     

典型农业流域不同类型池塘水体CO2排放特征

内陆水体是大气CO₂收支估算的重要组成部分。农业流域分布着大量池塘景观水体,且具备蓄洪抗旱、消纳污染、水产养殖等多种功能。但是,农业流域不同功能的小型池塘CO₂排放特征尚不清楚。本研究以极具农业流域代表性的烔炀河流域为研究对象,选取流域中用于水产养殖(养殖塘)、生活污水承纳(村塘)、农业灌溉(农塘)、蓄水(水塘)的4个功能不同的景观池塘,基于为期1年的野外实地观测,以明确农业流域小型池塘CO₂排放特征。结果表明,不同功能池塘水体CO₂排放差异显著,受养殖活动、生活污水输入和农田灌溉等人类活动影响,养殖塘((80.37±100.39) mmol/(m²·d))、村塘((48.69±65.89) mmol/(m²·d))和农塘((13.50±15.81) mmol/(m²·d))是大气CO₂的热点排放源,其CO₂排放通量分别是自然蓄水塘((4.52±23.26) mmol/(m²·d))的18、11和3倍。统计分析也表明,该流域池塘CO₂排放变化总体上受溶解氧、营养盐等因素驱动。4个不同景观池塘CO₂排放通量全年均值为(37.31±67.47) mmol/(m²·d),是不容忽视的CO₂排放源,其中养殖塘和村塘具有较高的CO₂排放潜力,在未来研究中需要重点关注。     

Riverine input and air–sea CO2 exchanges near the Changjiang (Yangtze River) Estuary: Status quo and implication on possible future changes in metabolic status

Due to anthropogenic activities, the nutrient loadings of the Changjiang (Yangtze River) are strickly on the rise. The high nutrient concentrations notwithstanding, river water was pCO₂ supersaturated in the inner estuary during summer 2003 but decreased quickly in the mid-estuary due to mixing with low pCO₂ waters from offshore. In addition, settling of particles in the estuary resulted in better light conditions so that phytoplankton bloomed, driving down pCO₂ to ∼200 μatm. In the outer estuary and outside of the bloom area, pCO₂ increased again to near or just below saturation. Literature data also reveal that the mainstream of the Changjiang is always supersaturated with respect to CO₂ probably because the decomposition of terrestrial organic matter overwhelms the consumption of CO₂ due to biological production.     

Capillary pressure for the sand–CO2–water system under various pressure conditions. Application to CO2 sequestration

Accurate modeling of storage of carbon dioxide (CO₂) in heterogeneous aquifers requires experiments of the capillary pressure as function of temperature and pressure. We present a method with which static drainage and imbibition capillary pressures can be measured continuously as a function of saturation at various temperature (T) and pressure (P) conditions. The measurements are carried out at (T, P) conditions of practical interest. Static conditions can be assumed as small injection rates are applied. The capillary pressure curves are obtained for the unconsolidated sand–distilled water–CO₂ system. The experimental results show a decrease of drainage and imbibition capillary pressure for increasing CO₂ pressures and pronounced dissolution rate effects for gaseous CO₂. Significant capillary pressure fluctuations and negative values during imbibition are observed at near critical conditions. The measurement procedure is validated by a numerical model that simulates the experiments.     

Feasibility of Monitoring the Hontomín (Burgos, Spain) CO2 Storage Site Using a Deep EM Source

Geophysical methods have been used experimentally during the last decade, a period of strong development, being adopted as complementary techniques for characterizing and monitoring hydrocarbon and gas reservoirs. In this study, we evaluated the ability of the controlled source electromagnetic (CSEM) method to monitor the storage of CO₂ at the Research Laboratory on Geological Storage of CO₂ at Hontomín (Burgos, Spain). Two aspects of the CSEM monitoring were examined considering the geoelectrical structure at the site, the technological constraints and the noise conditions of the Hontomín area. Borehole-to-surface simulations were performed to evaluate the detectability of the resistivity changes in the reservoir and the capacity to determine the location of the CO₂ plume. The synthetic time-lapse study explores the possibilities of CSEM monitoring with a deep electric source. Three depths of the source are analyzed: above the plume, inside the plume, and beneath the stored CO₂. In terms of the Hontomín storage site, the study confirmed that a deep electric source located beneath the injection depth can provide valuable information on the behavior of the stored CO_2.     

Interactions between gravity currents and convective dissolution

Geological storage of carbon dioxide (CO₂) is a promising technology for reducing atmospheric emissions. The large discrepancy in the time- and length-scales between up-dip migration of buoyant supercritical CO₂ and the sinking fingers of dissolved CO₂ poses a challenge for numerical simulations aimed at describing the fate of the plume. Hence, several investigators have suggested methods to simplify the problem, but to date there has been no reference solution with which these simplified models can be compared. We investigate the full problem of Darcy-based two-phase flow with gravity-current propagation and miscible convective mixing, using high-resolution numerical simulations. We build on recent developments of the Automatic Differentiation - General Purpose Research Simulator (AD-GPRS) at Stanford. The results show a CO₂ plume that travels for 5000 years reaching a final distance of 14 km up-dip from the injection site. It takes another 2000 years before the CO₂ is completely trapped as residual (40%) and dissolved (60%) CO₂. Dissolution causes a significant reduction of the plume speed. While fingers of dissolved CO₂ appear under the propagating gravity current, the resident brine does not become fully saturated with CO₂ anywhere under the plume. The overall mass transfer of CO₂ into the brine under the plume remains practically constant for several thousands of years. These results can be used as a benchmark for verification, or improvements, of simplified (reduced-dimensionality, upscaled) models. Our results indicate that simplified models need to account for: (i) reduced dissolution due to interaction with the plume, and (ii) gradual reduction of the local dissolution rate after the fingers begin to interact with the bottom of the aquifer.