Dissolution Flux Research Articles

Benthic contribution to seasonal silica budgets in two macrotidal estuaries in North-Western France

The paper aims to build seasonal silica budgets in two macrotidal estuaries, the Elorn and Aulne estuaries of the Bay of Brest (North-Western France), based on modeling and measurements, in order to increase our understanding of the silica (Si) cycle at land-sea interfaces. A diagenetic model was developed to quantify benthic Si fluxes, e.g. aSiO2 deposition fluxes that are difficult to assess through direct measurements. Sediment cores were also seasonally sampled at six stations to provide data essential to parametrize and validate the model. Vertical profiles of porosity, burrowing depth, biodiffusive coefficients, concentrations of amorphous silica (aSiO2) and silicic acid (Si(OH)4 and the proportion of reactive aSiO2 were measured. The results show that sites sampled along the Elorn and Aulne estuaries constitute significant net Si deposition areas (1-4.5 mmol Si m-2 d-1), particularly in the upstream during winter and in midstream and downstream during summer. Year round, reprecipitation is negligible (< 3%) while burial accounts for the retention of ~ 30-80% of deposited aSiO2. In winter, burial dominates the benthic Si budget. As surface-integrated benthic Si fluxes are low compared to riverine aSiO2 fluxes, the Si export to coastal waters is high (93%) during winter. In contrast, in summer, burial accounts for 38% of river Si fluxes, and Si(OH)4 flux from the sediment is high as a result of enhanced benthic recycling and bioirrigation. Internal estuarine processes, e.g., benthic and pelagic primary production, dissolution and benthic Si fluxes, surpass river fluxes in magnitude during summer. Overall, we conclude that the Elorn and Aulne macrotidal estuaries are efficient filters of Si, retaining about 4-38% of river Si fluxes, and even 6-67% when accounting for retention in intertidal marshes, but with massive exports occurring during winter floods.

Molecular phenomena related to moisture uptake in amorphous solid dispersion loaded with bosentan monohydrate and copovidone

Amorphous bosentan alone lacks dissolution flux that could enhance its bioavailability. Its coamorphization with hydrophilic copovidone (1:1) enables to improve wettability and dissolution rate, but fine amorphous particles are prone to moisture uptake. Water sorbed on the surface of this amorphous solid dispersion can considerably alter its physical properties annihilating benefits of coamorphization. The gravimetric measurements of water uptake, the solid state 1H NMR spectroscopy and relaxometry enabled us to describe for the first time, phase changes initiated by hydration in amorphous bosentan systems. The properties of copovidone greatly impacted water uptake in bosentan solid dispersions. A nonlinear reduction of the Tg upon water sorption resulted in the transformation of the glassy state into the rubbery state at ambient temperature. The state diagrams were developed for optimization of manufacturing conditions, selection of suitable packaging material and storage temperature, ensuring long-term stability of amorphous bosentan products.

Numerical Investigation of the Influence of Hydrodynamic Dispersion on Solutal Natural Convection

AbstractWe investigate numerically the effect of hydrodynamic dispersion on convective dissolution of carbon dioxide in saline aquifers. Solutions of the transport equations were used to describe the dissolution process in the aquifer and provide a systematic parametric analysis of the influence of dispersion on two important measures of convective dissolution, the wavenumber, and dissolution flux. The results suggest that dispersion decreases the dissolution rate and reduces the finger wavenumber. Based on the simulated results, new empirical scaling laws that predict the dissolution rate and wavenumber were developed. The application of the new laws to two storage sites shows that the currently available predictions overestimate the dissolution rates by ∼30%. We have identified some discrepancies between published scaling laws that were obtained for the dissolution rate. While most numerical studies identify a linear scaling, experimental investigations often suggest a sublinear behavior. Our findings resolve the controversy by suggesting that dispersion, which was not considered in these past numerical studies, is the reason for the apparent sublinear scaling.

Drug Release from Carrier Systems Comprising Meloxicam Crystals Formed by Impregnation-Evaporation

The impregnation of poorly water-soluble drug onto the surface of a suitable pharmaceutical excipient, used as a hydrophilic carrier, can lead to the preparation of systems with improved dissolution properties due to the separation of drug crystal particles on the carrier surface. For this purpose, a method based on impregnation of hydrophilic matrix by the hydrophobic poorly water-soluble drug Meloxicam (MX) solution in volatile organic solvent was used. After the evaporation of the solvent, the method resulted in coverage of the carrier surface by drug crystals. The influence of the amount and concentration of the impregnating solution on the formed MX crystal size and the dissolution rate was evaluated. Firstly, the impregnation forming crystals on the planar surface was studied and the MX maximum dissolution flux from that surface was determined. The optimum preparation method was further used to produce a volume of impregnated granules. The dissolution performance of the granules was evaluated, and the dissolution kinetics was described by mathematical models. The polymorphic modification of impregnated API and influence of impregnated drug amount on the hydrophilic carrier surface coverage were considered. From the results of this work, it is clear that the impregnated drug amount and the number of impregnations cycles can be optimized to achieve maximum drug release rate.

Numerical simulation of density-driven non-Newtonian fluid flow

Abstract Density-driven flow is numerically studied. The sinking fluid is set as a power-law non-Newtonian fluid with a higher density than the environmental fluid. During the simulation process, saturation concentration is fixed on the upper boundary; thus downward plumes are formed because of gravitational instability. The dissolution flux undergoes a series of changes, from the initially diffusion-dominated regime to the convection-dominated regime due to the appearance of finger structures, and then to the transition of finger structures merging into larger plumes. Finally, it enters the shutdown regime as the plumes start to reach the impermeable bottom boundary. In the process of plume sinking, different fluid properties have an important impact on the downward velocity, shape of plumes and the dissolution flux of the flow field. The tip velocity of the plumes is slowed until the high-concentration fluid is supplied to further push the plumes downward. For the shear-thinning fluid ambient fluid, this phenomenon is even more drastic. However, for shear-thickening fluid, this phenomenon is almost not observed. In addition, unlike the condition of a Newtonian fluid, protoplumes on the original interface appear at the early stage. Prominent protoplumes have developed between the primary plumes in non-Newtonian fluids throughout the entire process.

Numerical Simulation of Carbon Dioxide–Nitrogen Mixture Dissolution in Water-Saturated Porous Media: Considering Cross-Diffusion Effects

The possibility of impure carbon dioxide (CO2) sequestration can reduce the cost of these projects and facilitate their widespread adoption. Despite this, there are a limited number of studies that address impure CO2 sequestration aspects. In this study, we examine the convection–diffusion process of the CO2–nitrogen (N2) mixture dissolution in water-saturated porous media through numerical simulations. Cross-diffusion values, as the missing parameters in previous studies, are considered here to see the impact of N2 impurity on dissolution trapping in more realistic conditions. Homogeneous porous media are used to examine this impact without side effects from the heterogeneity, and then simulations are extended to heterogeneous porous media, which are a good representative of the real fields. Heterogeneity in the permeability field is generated with sequential Gaussian simulation. Using the averaged dissolved CO2 and dissolution fluxes for each case, we could determine the onset of different dissolution regimes and behaviors of dissolution fluxes in CO2–N2 mixture dissolution processes. The results show that there is a notable difference between the pure cases and impure cases. Additionally, a failure to recognize the changes in the diffusion matrix and cross-diffusion effects can result in significant errors in the dissolution process. At lower temperatures, the N2 impurity decreases the amount and flux of CO2 dissolution; however, at higher temperatures, sequestrating the CO2–N2 mixture would be a more reasonable choice due to enhancing the dissolution behavior and lowering the project costs. The results of the heterogeneous cases indicate that heterogeneity, in most cases, reduces the averaged dissolved CO2, and dissolution flux and impedes the onset of convection. We believe that the results of this study set a basis for future studies regarding the CO2–N2 mixture sequestration in saline aquifers.

Pore-scale study of convective mixing process in brine sequestration of impureCO2

The present study investigates the effects of impurities on convective mixing processes in geological sequestration of CO${}_{2}$ at pore scale. We focus on the concentration expansion coefficient and diffusion rate of different impurities, the effects of which on the fingering phenomena, dissolution flux, as well as the onset time of convection ${t}_{o\phantom{\rule{0}{0ex}}n}$ are mainly analyzed. Based on the numerical results, the mathematical form of effective Rayleigh number Ra${}_{e}$ in a multicomponent system is fit, which could ensure that the scaling relations between ${t}_{o\phantom{\rule{0}{0ex}}n}$ and Ra${}_{e}$ are consistent with that in a pure system.

Convective dissolution of carbon dioxide in two- and three-dimensional porous media: The impact of hydrodynamic dispersion

Convective dissolution is the process by which CO2 injected in geological formations dissolves into the aqueous phase and thus remains stored perennially by gravity. It can be modeled by buoyancy-coupled Darcy flow and solute transport. The transport equation should include a diffusive term accounting for hydrodynamic dispersion, wherein the effective diffusion coefficient is proportional to the local interstitial velocity. We investigate the impact of the hydrodynamic dispersion tensor on convective dissolution in two-dimensional (2D) and three-dimensional (3D) homogeneous porous media. Using a novel numerical model, we systematically analyze, among other observables, the time evolution of the fingers' structure, dissolution flux in the quasi-constant flux regime, and mean concentration of the dissolved CO2; we also determine the onset time of convection, ton. For a given Rayleigh number Ra, the efficiency of convective dissolution over long times is controlled by ton. For porous media with a dispersion anisotropy commonly found in the subsurface, ton increases as a function of the longitudinal dispersion's strength (S), in agreement with previous experimental findings and in contrast to previous numerical findings, a discrepancy that we explain. More generally, for a given strength of transverse dispersion, longitudinal dispersion always slows down convective dissolution, while for a given strength of longitudinal dispersion, transverse dispersion always accelerates it. Furthermore, a systematic comparison between 2D and 3D results shows that they are consistent on all accounts, except for a slight difference in ton and a significant impact of Ra on the dependence of the finger number density on S in 3D.

Scaling CO2 convection in confined aquifers: Effects of dispersion, permeability anisotropy and geochemistry

Solubility trapping of carbon dioxide (CO2) in deep saline aquifers is considered an effective mechanism of carbon storage. The dissolution of CO2 in aquifer brine may result in gravitational instability, which triggers convective mixing (similar to the well-known Rayleigh–Bénard convection problem). The process starts with the diffusion of CO2 into the brine, followed by the onset of convection (tc), which may be followed by the constant-flux regime, F=Fc, where F is the dissolution flux. Scaling tc and Fc with characteristic measures (such as Rayleigh number as a measure of buoyancy to diffusive driving forces) is important for the characterization of CO2 injection at a large scale. Previously, natural complexities such as hydrodynamic dispersion, permeability anisotropy and geochemical interactions have been neglected in the scaling relations of convective mixing. This work explores the effects of such simplifications on the scaling relations of convective mixing using high-resolution 2D numerical simulations. Our results provide new insights from revisiting the convective mixing scaling. We show that the Sherwood number (Sh) depends on the domain height in the presence of the hydrodynamic dispersion. In line with such findings, we show that Sh-Rayleigh scaling prefactor is directly related to longitudinal dispersivity (αL). Moreover, we show that increasing the permeability in each direction is beneficial for the process by decreasing convection onset time (tc) and increasing the dissolution flux (F). Smaller permeability anisotropy ratio (defined as the ratio of vertical to horizontal permeability, ℘=Kz/Kx) results in earlier onset time and higher dissolution flux, which scales with ℘0.54 and ℘−0.21 compared to convection–diffusion, respectively. Finally, our simulation results show that earlier tc and higher F are expected due to carbonate geochemical reactions. The scaling relations of convective mixing in deep saline aquifers guide prioritization and selection of appropriate aquifers for geological CO2storage and designing efficient injection schemes.

Effect of permeability heterogeneity on the dissolution process during carbon dioxide sequestration in saline aquifers: two-and three-dimensional structures

The convection–diffusion process of carbon dioxide (CO2) dissolution in a saline reservoir is investigated to shed light on the effects of the permeability heterogeneity. Using sequential Gaussian simulation method, random permeability fields in two and three-dimension (2D and 3D) structures are generated. Quantitative (average amount of the dissolved CO2 and dissolution flux) and qualitative (pattern of the dissolved CO2 and velocity streamlines) measurements are used to investigate the results. A 3D structure shows a slightly higher dissolution flux than a 2D structure in the homogeneous condition. Results in the random permeability fields in 2D indicates an increase in the standard deviation of the permeability nodes enhances the dissolution efficiency, fluctuations in CO2 dissolution flux, separation between the different realizations from the same input parameters, and tendency toward more jagged convective fingers’ shape. Furthermore, the distance between the permeability nodes increases the convective fingers’ dissolution efficiency and jagged structure. The degree of freedom in 3D structures results in a higher chance of escaping from the low permeability zones and reduces the interactions between convective fingers in 3D systems. With the same variance and correlation length between permeability nodes, connectivity between high permeable zones in 3D cases are less than that of 2D cases; therefore, 2D realizations overestimate the dissolution flux of real heterogeneous 3D structures, which should be considered carefully.Article HighlightsCO2 sequestration in two and three dimensional heterogeneous saline aquifers are investigated.3D structures in homogeneous conditions show higher dissolution than 2D structures.2D realizations overestimates the dissolution flux over real heterogeneous 3D reservoirs.

Food effect risk assessment in preformulation stage using material sparing μFLUX methodology.

The intake of food and meal type can strongly impact the bioavailability of orally administered drugs and can consequently impact drug efficacy and safety. During the early stages of drug development, only a small amount of drug substance is available, and the solubility difference between fasted state simulated intestinal fluid and fed state simulated intestinal fluid may provide an early indication about the probable food effect. But higher drug solubility in fed state simulated intestinal fluid may not always results in an increased oral absorption. In the present research, we demonstrated using 11 model compounds that in addition to the drug dissolution in biorelevant media, the evaluation of the diffusion flux of a drug in solution, across artificial lipid coated membrane, where only the unbound drug crosses the membrane, is a reliable way to predict the food effect. Although, the combination of dissolution and diffusion flux may not reliably predict the food effect in case of drugs undergoing intestinal metabolism or when transporters are involved in the drug absorption, the technique generally provides good information about the food effect at very early stages of drug development that may help in designing a clinical plan by adjusting the drug dose in the fed state.

Site-specific interactions enhanced dissolution of natural aragonite (110) surfaces in succinic acid (SUC) solutions: Implications for the oceanic aragonite dissolution fluxes

Aragonite, one of the most common biological calcium carbonate minerals, is widespread in marine plankton and neritic sediments (e.g., accounting for 89% of pelagic calcification of CaCO3 in the surface ocean). Its dissolution directly affects the export fluxes of CaCO3 in seawater. The aragonite dissolution in the ocean correlates with the increase of partial pressure of carbon dioxide and is pertinent to acidic biomolecules. However, aragonite dissolution in seawater with acidic biomolecules has been overlooked, and the interaction mechanism is unclear. In-situ atomic force microscopy (AFM) was employed to observe the dissolution features of aragonite (110) growth surfaces in succinic acid (SUC, HOOC-CH2-CH2-COOH) solutions. The results demonstrate that (1) both the morphologies and spreading rates of the etch pits formed on aragonite (110) surfaces are altered by the interactions between SUC molecules and the surfaces; (2) the [11‾1] and [1‾11] steps of the etch pits on aragonite (110) surfaces in SUC solutions are kinetically controlled; (3) dissolution rates of aragonite (110) surfaces are proportional to SUC concentrations, which is attributed to the strong complexation between SUC molecules and surface-bounded Ca atoms (≡Ca+); (4) etch pits morphologies of aragonite (110) and calcite (10.4) surfaces are different in SUC solutions, and the spreading rates of the etch pits of the former are one to two orders of magnitude lower than those of the latter. Furthermore, aragonite is found to be more sensitive to SUC molecules than calcite, suggesting that dissolving aragonitic materials could be more easily affected by circumambient biomolecules than dissolving calcitic materials. In seawater that contains organic molecules, the dissolution fluxes of aragonite could be much slower than those of calcite. These findings not only reveal the site-specific interactions between SUC molecules and the ≡Ca+ on aragonite (110) surfaces but also emphasize its implication for the oceanic aragonite dissolution fluxes.

Modulating carbon growth kinetics enables electrosynthesis of graphite derived from CO2 via a liquid–solid–solid process

Highly graphitic carbon materials have gained considerable interests in practical applications, however, an efficient and cost-effective synthesis strategy using low-grade carbonaceous precursors is still in urgent need. In this work, we successfully synthesize well-crystalline graphite derived from CO2 by molten carbonate electrolysis under a mild operating temperature, where the as-formed carbon atoms follow a “dissolution–precipitation” process on a Ni cathode. Attributed to that Ni cathode can in situ act as a solid solvent for periodically accommodating/dissolving the as-formed carbon atoms, deliberately coordinating carbon formation flux with carbon dissolution flux can lead to the consecutive production of highly crystalline graphite, without contamination of transition metal catalyst. It was found that a low carbon deposition current density and a relatively high operating temperature (650–750 °C) both facilitate the growth of graphite structures, because a moderate current density enables a suitable carbon flux originating from the electro-reduction of the captured CO2 (in the form of CO32− in molten salts), which can more accessibly match the carbon dissolution flux in Ni substrate at an elevated temperature. The thickness of graphite can be easily controlled by electrolysis durations. This work provides a simple strategy to convert CO2 into graphitic carbon products with both promising purity and crystallinity.

Mass Flux Analysis of Abiotic Tetrachloroethene Dense Nonaqueous Phase Liquid Pool Dissolution in a Heterogeneous Flow Environment

AbstractPorous aquifer materials are often characterized by layered heterogeneities that influence groundwater flow and present complexities in contaminant transport modeling. Such flow variations also have the potential to impact the dissolution flux from dense nonaqueous phase liquid (DNAPL) pools. This study examined how these heterogeneous flow conditions affected the dissolution of a tetrachloroethene (PCE) pool in a two‐dimensional intermediate‐scale flow cell containing coarse sand. A steady‐state mass‐balance approach was used to calculate the PCE dissolution rate at three different flow rates. As expected, aqueous PCE concentrations increased along the length of the PCE pool and higher flow rates decreased the aqueous PCE concentration in the effluent. Nonreactive tracer studies at two flow rates confirmed the presence of a vertical flow gradient, with the most rapid velocity located at the bottom of the tank. These results suggest that flow focusing occurred near the DNAPL pool. Effluent PCE concentrations and pool dissolution flux rates were compared to model predictions assuming local equilibrium (LE) conditions at the DNAPL pool/aqueous phase interface and a uniform distribution of flow. The LE model did not describe the data well, even over a wide range of PCE solubility and macroscopic transverse dispersivity values. Model predictions assuming nonequilibrium mass‐transfer‐limited conditions and accounting for vertical flow gradients, however, resulted in a better fit to the data. These results have important implications for evaluating DNAPL pool dissolution in the field where subsurface heterogeneities are likely to be present.

Spreading and mixing during solutal convection in uniform porous media with application to geologic CO2 storage

Convective dissolution in saline aquifers is expected to positively impact subsurface storage of carbon dioxide (CO2) by accelerating its dissolution rate into reservoir brines. By largely focusing on the dissolution flux, previous studies lack a systematic evaluation of the mixing process following CO2 emplacement, including a quantitative analysis at conditions representative of subsurface traps (Rayleigh number, Ra≤1 000). Here, we investigate solutal convection numerically in a two-dimensional uniform porous medium in the regime Ra=100−10 000. The macroscopic evolution of the convective process is characterized by means of fundamental macroscopic measures of mixing that use the local spatial structure of the solute concentration field. It is shown that the intensity of segregation closely mimics the evolution of the in situ convective pattern arising from the stretching and merging of downwelling plumes. The spreading length and the dilution index both confirm that the mixing process accelerates over time (t) with a power law scaling (∝tα) that transitions from diffusive (α=0.5) to superdiffusive mixing (α≥1) irrespective of Ra. This transition time scales τon∝Ra−2 and is used as a measure of the onset time of convection. The dilution index indicates that the time needed to reach close-to-complete mixing reduces linearly with Ra. On the contrary, the non-dimensional mass flux, expressed in terms of the Sherwood number, Sh, reveals a natural logarithmic scaling for Ra≤2 500.

Flux and pathway of iodine dissolution from brackish lake sediment in the northeast of Japan

Sediment is one of the most important entities controlling the environmental dynamics of iodine. We previously evaluated the dissolution flux of iodine from aquatic sediment to its overlying water in a brackish lake through an incubation experiment with a sediment core sample, reporting the regulation factors of this flux, such as the temperature and oxygenic conditions. In this study, factors controlling the seasonal variation in the dissolution flux of iodine were investigated via an incubation experiment using the sediment core samples collected in autumn and summer. The dissolution flux in this study was significantly smaller than that reported in our previous study. The iodine concentration detected in the overlying water of the sediment during incubation in this study was positively correlated with the concentrations of some inorganic ions, such as Na+, Cl−, and SiO42−, while these correlations were not confirmed in our previous study. As the dissolution of sedimentary iodine includes two pathways, which are the diffusion of sedimentary pore water and degradation of organic matter on surface sediment, correlations potentially indicate that the dissolution flux estimated in this study has a larger contribution from sedimentary pore water than that in our previous study. In addition, the higher flux estimated in our previous study was considered to be caused by the larger contribution from iodine derived from the degradation of phytoplanktonic organic matter on surface sediment. Assuming that the dissolution fluxes estimated in the previous and present studies are representative of the fluxes during and excluding the high productivity season in Lake Obuchi, respectively, we estimated the annual flux at 2.7 g y−1 m−2, which is comparable with our previous estimation.

Convective carbon dioxide dissolution in a closed porous medium at high-pressure real-gas conditions

We combine modeling and measurements to investigate the dynamics of convective carbon dioxide (CO2) dissolution in a pressure-volume-temperature cell, extending a recent study by Wen et al. (J. Fluid Mech., vol. 854, 2018, pp. 56–87) at low-pressure under ideal-gas conditions to high-pressure and real-gas conditions. Pressure-dependent compressibility and solubility are included to model the evolution of CO2 concentration in the gas phase and at the interface, respectively. Simple ordinary-differential-equation models are developed to capture the mean behavior of the convecting system at large Rayleigh number and are then verified by using both numerical simulations and laboratory experiments. The prefactor for the linear scaling of convective CO2 dissolution is evaluated – for the first time – by using pressure-decay experiments in bead packs at reservoir conditions. The results show that our models could quantitatively predict the process of the convective CO2 dissolution in pressure-decay experiments. Moreover, the results also reveal that for increasing gas pressure in closed systems, the negative feedback of the pressure drop – resulting from the dissolution of CO2 in the liquid – is weakened due to the decrease of the solubility constant at real-gas conditions. Our analysis provides a new direction for determination and validation of the convective dissolution flux of CO2 in porous media systems.

Diffusion coefficients of CO2–SO2–water and CO2–N2–water systems and their impact on the CO2 sequestration process: Molecular dynamics and dissolution process simulations

AbstractThe high cost of the CO2 sequestration in saline aquifers is a barrier to the implementation of them. However, a large portion of the cost is invested to purify and transport the CO2 from the flue gas stream of the emission sources. Therefore, the possibility of injecting impure CO2 will reduce the costs strongly. The diffusion coefficient is an important factor that plays a significant role in different aspects of the process. In spite of its importance, it is got less attention due to complex experimental procedures and low range of temperature and pressure applicability in the experimental conditions. To shed light on the effects of the impurity on the diffusion coefficient of CO2‐water systems, two types of impurities (SO2 and N2) in two levels are considered in this study through the molecular dynamics simulation approach. Simulations are done on a wide range of pressure and temperature conditions to cover a wide range of operational conditions for CO2 sequestration projects. The outcomes of these simulations were used in the direct numerical simulations to analyze the effect of the diffusion coefficient matrix changes on the CO2 dissolution process such as dissolution flux, the motion and shape of convective fingers, and their patterns. Results indicate that impurity has a great impact on the diffusion coefficient, and consequently on the CO2 dissolution behavior. We hope that reported results will pave the way for future studies regarding impure CO2 sequestration in saline aquifers. © 2021 Society of Chemical Industry and John Wiley & Sons, Ltd.

Effect of Argon Flow on Oxygen and Carbon Coupled Transport in an Industrial Directional Solidification Furnace for Crystalline Silicon Ingots

Transient global simulations were carried out to investigate the effect of argon flow on oxygen and carbon coupled transport in an industrial directional solidification furnace for quasi-single crystalline silicon ingots. Global calculation of impurity transport in the argon gas and silicon melt was based on a fully coupled calculation of the thermal and flow fields. Numerical results show that the argon flow rate affects the flow intensity along the melt–gas surface, but has no significant effect on the flow patterns of silicon melt and argon gas above the melt–gas surface. It was found that the evaporation flux of SiO along the melt–gas surface decreases with the increasing argon flow rate during the solidification process. However, the net flux of oxygen atoms (SiO evaporation flux minus CO dissolution flux) away from the melt–gas surface increases with the increasing argon flow rate, leading to a decrease in the oxygen concentration in the grown ingot. The carbon concentration in the grown ingot shows an exponential decrease with the increase of the argon flow rate, owing to the fact that the dissolution flux of CO significantly decreases with the increasing argon flow rate. The numerical results agree well with the experimental measurements.

Dynamics of CO2 Density‐Driven Flow in Carbonate Aquifers: Effects of Dispersion and Geochemistry

AbstractThe dissolution of carbon‐dioxide (CO2) in deep saline aquifers is an important trapping mechanism in carbon storage. This process is triggered by unstable high‐density CO2 front, which later promotes density‐driven mixing, hydrodynamic dispersion of CO2, and favors the long‐term sequestration. In many former studies, effects of hydrodynamic dispersion and multispecies geochemical reactions have been ignored. This work elaborates the impacts of these simplifications on the dynamics of convective mixing by numerical simulations. Geochemical effects were studied by the implementation of rock‐fluid and fluid‐fluid interactions for a typical carbonate aquifer. Results show that accounting for the hydrodynamic dispersion decreases the convection onset time and increases the CO2 dissolution flux, which is more significant in larger dispersivities and Rayleigh numbers. Results indicate that carbonate geochemical reactions intense the long‐term overall efficiency of the process, while decrease the total amount of sequestered carbon in the diffusion‐dominated period. Results also reinforce the importance of realistic geochemical representation and importance of spatial and temporal dependence of the reactions pathway, subsequent to the finger development for more detailed simulation of the CO2 storage process.