Impact of pressure, salt concentration, and temperature on the convective dissolution of carbon dioxide in aqueous solutions

Loodts, Vanessa; Rongy, Laurence; Wit, A. De

doi:10.1063/1.4896974

Cited by 44 publications

(67 citation statements)

References 47 publications

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“…When R A > 0, in case 1a, A increases the density of the solution upon dissolution, which leads to a denser zone rich in A above the less dense host bulk solvent [16][17][18][19]44 . In case 1b, A decreases the density of the solution upon dissolution so that a less dense zone rich in A forms below the denser host bulk solvent.…”

Section: Classification Of Reaction-diffusion Density Profilesmentioning

confidence: 99%

“…We assume a local equilibrium at the interface located at z = 0 so that the concentration of A at the interface is always equal to its solubility A 0 in the host phase, which may depend on experimental parameters (temperature, salinity, pressure, ...) 19 and is not limited by diffusion. We assume that the volume of the host phase does not change significantly upon dissolution of A and do not consider any thermal 29,41 or dispersion effects 42 .…”

Section: Description Of the Physical Modelmentioning

confidence: 99%

“…When CO 2 is injected in geological sites, it dissolves into a host liquid phase (oil or water), increasing thereby its density, which results in a buoyantly unstable density stratification. The contact zone between the denser CO 2 -rich and the less dense bulk solution layers is then destabilized in the form of buoyancy-driven fingering [10][11][12][14][15][16][17][18][19] . It is of current interest to characterize this dissolution-driven convective instability as it contributes to the mechanism of CO 2 sequestration known as "solubility trapping" 15 .…”

Section: Introductionmentioning

confidence: 99%

“…Studies have reported the impact on these properties of boundary conditions 21,22,28 , anisotropy of the permeability 16,[23][24][25]28 , geometry of the system 26 , compressibility and interface movement 27 , a geothermal gradient 28,29 , and control parameters in laboratory experiments 5,[10][11][12]19 . However, an important aspect that has been less investigated is the impact of chemical reactions on such instabilities.…”

Section: Introductionmentioning

confidence: 99%

“…In particular, the early-stage development of this instability has been characterized both theoretically and experimentally for porous media or Hele-Shaw cells with a focus on the critical time and wavenumber for the onset of convection 5,[10][11][12]16,[18][19][20][21][22][23][24][25][26][27][28][29] . Studies have reported the impact on these properties of boundary conditions 21,22,28 , anisotropy of the permeability 16,[23][24][25]28 , geometry of the system 26 , compressibility and interface movement 27 , a geothermal gradient 28,29 , and control parameters in laboratory experiments 5,[10][11][12]19 .…”

Section: Introductionmentioning

confidence: 99%

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Chemical control of dissolution-driven convection in partially miscible systems: theoretical classification

Loodts

Rongy

Wit

2015

Phys. Chem. Chem. Phys.

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Dissolution-driven convection occurs in the host phase of a partially miscible system when a buoyantly unstable density stratification develops upon dissolution. Reactions can impact such convection by changing the composition and thus the density of the host phase. Here we study the influence of A+B→ C reactions on such convective dissolution when A is the dissolving species and B a reactant initially present in the host phase. We perform a linear stability analysis of related reaction-diffusion density profiles to compare the growth rate of the instability in the reactive case to its non reactive counterpart when all species diffuse at the same rate. We classify the stabilizing or destabilizing influence of reactions on the buoyancy-driven convection in a parameter space spanned by the solutal Rayleigh numbers R A,B,C of chemical species A, B, C and by the ratio β of initial concentrations of the reactants. For R A > 0, the non reactive dissolution of A in the host phase is buoyantly unstable. In that case, we show that reaction is enhancing convection provided C is sufficiently denser than B. Increasing the ratio β of initial reactant concentrations increases the effect of chemistry but does not significantly impact the stabilizing/destabilizing classification. When the non reactive case is buoyantly stable (R A < 0), reactions can create in time an unstable density stratification and trigger convection if R C > R B . Our theoretical approach allows classifying previous results in a unifying picture and developing strategies for chemical control of convective dissolution.

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Section: Classification Of Reaction-diffusion Density Profilesmentioning

confidence: 99%

Section: Description Of the Physical Modelmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Chemical control of dissolution-driven convection in partially miscible systems: theoretical classification

Loodts

Rongy

Wit

2015

Phys. Chem. Chem. Phys.

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Linear and nonlinear analyses of the effect of chemical reaction on the onset of buoyancy‐driven instability in a CO₂ absorption process in a porous medium or Hele‐Shaw cell

Kim

Wylock

2016

Can J Chem Eng

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To understand CO2 absorption into a basic solution saturated porous medium or a Hele‐Shaw cell, the effect of the chemical reaction between dissolved CO2 and the basic reactant in the solution on the onset of a buoyancy‐driven instability in a gas absorption process is analyzed theoretically. For the infinitely fast reaction, new linear and non‐linear stability equations are derived without the quasi‐steady state assumption (QSSA) and solved analytically. The present stability analysis without the QSSA shows that the important parameters are the dimensionless densification numbers and the reactant concentration ratio. For the physically unstable system, the chemical reaction can induce a non‐monotonic density profile and has an important effect on the onset of instability motion. The effect of the reactant concentration ratio on the stability of the system is strongly dependent on the physical situation. Here, we call the system which is physically stable when there is no chemical reaction as the physically stable system. Even for this physically stable system, the chemical reaction makes the system unstable and induces the gravitational fingering instability motion. Also, it is found that the stability of the physically stable system is relatively insensitive to the non‐monotonicity of the density profile.

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Prerequisites for density-driven instabilities and convective mixing under broad geological CO2 storage conditions

Rasmusson

Fagerlund

Tsang

et al. 2015

Advances in Water Resources

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Prerequisites for density-driven instabilities and convective mixing under broad geological CO 2 storage conditions, Advances in Water Resources (2015), Highlights We develop an instability onset, onset time and steady convective flux-analysis tool.  A systematic analysis of prerequisites for enhanced solubility trapping is presented.  Indirect thermal effects on enhanced solubility trapping are non-negligible.  Shallow storage depths favor density-driven instability onset and short onset times.  Salinity determines the storage depth at which the largest convective fluxes occur. AbstractDirect atmospheric greenhouse gas emissions can be greatly reduced by CO 2 sequestration in deep saline aquifers. One of the most secure and important mechanisms of CO 2 trapping over large time scales is solubility trapping. In addition, the CO 2 dissolution rate is greatly enhanced if density-driven convective mixing occurs. We present a systematic analysis of the prerequisites for density-driven instability and convective mixing over the broad temperature, pressure, salinity and permeability conditions that are found in geological CO 2 storage. The onset of instability (Rayleigh-Darcy number, ), the onset time of instability and the steady convective flux are comprehensively calculated using a newly developed analysis tool that accounts for the thermodynamic and salinity dependence on solutally and thermally induced density change, viscosity, molecular and thermal diffusivity. Additionally, the relative influences of field characteristics are analysed through local and global sensitivity analyses.The results help to elucidate the trends of the , onset time of instability and steady convective flux under field conditions. The impacts of storage depth and basin type (geothermal gradient) are also explored and the conditions that favour or hinder enhanced solubility trapping are identified. Contrary to previous studies, we conclude that the geothermal gradient has a non-negligible effect on density-driven instability and convective mixing when considering both direct and indirect thermal effects because cold basin conditions, for instance, render higher compared to warm basin conditions. We also show that the largest is obtained for conditions that correspond to relatively shallow depths, measuring approximately 800 m, indicating that CO 2 storage at such depths favours the onset of density-driven instability and reduces onset times. However, shallow depths do not necessarily provide conditions that generate the largest steady convective fluxes; the salinity determines the storage depth at which the largest steady convective fluxes occur.

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Impact of pressure, salt concentration, and temperature on the convective dissolution of carbon dioxide in aqueous solutions

Cited by 44 publications

References 47 publications

Chemical control of dissolution-driven convection in partially miscible systems: theoretical classification

Chemical control of dissolution-driven convection in partially miscible systems: theoretical classification

Linear and nonlinear analyses of the effect of chemical reaction on the onset of buoyancy‐driven instability in a CO₂ absorption process in a porous medium or Hele‐Shaw cell

Prerequisites for density-driven instabilities and convective mixing under broad geological CO2 storage conditions

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Impact of pressure, salt concentration, and temperature on the convective dissolution of carbon dioxide in aqueous solutions

Cited by 44 publications

References 47 publications

Chemical control of dissolution-driven convection in partially miscible systems: theoretical classification

Chemical control of dissolution-driven convection in partially miscible systems: theoretical classification

Linear and nonlinear analyses of the effect of chemical reaction on the onset of buoyancy‐driven instability in a CO2 absorption process in a porous medium or Hele‐Shaw cell

Prerequisites for density-driven instabilities and convective mixing under broad geological CO2 storage conditions

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Linear and nonlinear analyses of the effect of chemical reaction on the onset of buoyancy‐driven instability in a CO₂ absorption process in a porous medium or Hele‐Shaw cell