“…An increase in siderite content or the presence of Fe oxides could not be identified in current experiments in XRD, although~11% of an amorphous phase was identified. Siderite formation has been predicted in simulations of the Ketzin pilot site for CO 2 storage, and in the Altensalzwedel gas reservoir, Germany, with siderite precipitation rather than ankerite predicted in Utsira reservoir, Norway (De Lucia et al, 2012;Klein et al, 2013;Pham et al, 2011).…”
Section: Co 2 -Water Reaction Of Siderite-ankeritementioning
“…An increase in siderite content or the presence of Fe oxides could not be identified in current experiments in XRD, although~11% of an amorphous phase was identified. Siderite formation has been predicted in simulations of the Ketzin pilot site for CO 2 storage, and in the Altensalzwedel gas reservoir, Germany, with siderite precipitation rather than ankerite predicted in Utsira reservoir, Norway (De Lucia et al, 2012;Klein et al, 2013;Pham et al, 2011).…”
Section: Co 2 -Water Reaction Of Siderite-ankeritementioning
“…The database minteq.v4.dat with the classic Debye-Hückel model for the calculation of the activity coefficient is thus used for all the subsequent simulations, despite its inadequacy for high salinity conditions. This is a recurrent issue for people working in high salinity systems, as stated in other studies (De Lucia et al, 2012).…”
-The sorption of inorganic elements on carbonate minerals is well known in strictly controlled conditions which limit the impact of other phenomena such as dissolution and/or precipitation. In this study, we evidence the behavior of Zn(II) (initially in solution) and two trace elements, Mn(II) and Sr(II) (released by carbonate dissolution) in the context of a leakage from a CO 2 storage site. The initial pH chosen are either equal to the pH of the water-CO 2 equilibrium (~2.98) or equal to the pH of the water-CO 2 -calcite system (~4.8) in CO 2 storage conditions. From this initial influx of liquid, saturated or not with respect to calcite, the batch experiments evolve freely to their equilibrium, as it would occur in a natural context after a perturbation. The batch experiments are carried out on two natural carbonates (from Lavoux and St-Emilion) with P CO 2 = 10 À3.5 bar, with different initial conditions ([Zn(II)] i from 10 À4 to 10 À6 M, either with pure water or 100 g/L NaCl brine). The equilibrium regarding calcite dissolution is confirmed in all experiments, while the zinc sorption evidenced does not always correspond to the two-step mechanism described in the literature. A preferential sorption of about 10% of the concentration is evidenced for Mn(II) in aqueous experiments, while Sr(II) is more sorbed in saline conditions. This study also shows that this preferential sorption, depending on the salinity, is independent of the natural carbonate considered. Then, the simulations carried out with PHREEQC show that experiments and simulations match well concerning the equilibrium of dissolution and the sole zinc sorption, with log K Zn(II)~2 in pure water and close to 4 in high salinity conditions. When the simulations were possible, the log K values for Mn(II) and Sr(II) were much different from those in the literature obtained by sorption in controlled conditions. It is shown that a new conceptual model regarding multiple Trace Elements (TE) sorption is required, to enable us to better understand the fate of contaminants in natural systems.
“…The storage in saline aquifer is actually an unfavourable case for the one-way coupling, given the complexity of its hydrodynamics; the case of CO 2 storage in depleted gas reservoirs would be much easier, where the water phase is typically present only in limited amount or residual saturations (Audigane et al, 2009;De Lucia et al, 2012). In such cases the hypothesis of self-similarity of reactions will be met to an even better extent, since the solute transport in the formation brine will be quite reduced, if present at all.…”
Abstract. Fully coupled, multi-phase reactive transport simulations of CO 2 storage systems can be approximated by a simplified one-way coupling of hydrodynamics and reactive chemistry. The main characteristics of such systems, and hypotheses underlying the proposed alternative coupling, are (i) that the presence of CO 2 is the only driving force for chemical reactions and (ii) that its migration in the reservoir is only marginally affected by immobilisation due to chemical reactions. In the simplified coupling, the exposure time to CO 2 of each element of the hydrodynamic grid is estimated by non-reactive simulations and the reaction path of one single batch geochemical model is applied to each grid element during its exposure time. In heterogeneous settings, analytical scaling relationships provide the dependency of velocity and amount of reactions to porosity and gas saturation. The analysis of TOUGHREACT fully coupled reactive transport simulations of CO 2 injection in saline aquifer, inspired to the Ketzin pilot site (Germany), both in homogeneous and heterogeneous settings, confirms that the reaction paths predicted by fully coupled simulations in every element of the grid show a high degree of self-similarity. A threshold value for the minimum concentration of dissolved CO 2 considered chemically active is shown to mitigate the effects of the discrepancy between dissolved CO 2 migration in non-reactive and fully coupled simulations. In real life, the optimal threshold value is unknown and has to be estimated, e.g. by means of 1-D or 2-D simulations, resulting in an uncertainty ultimately due to the process de-coupling. However, such uncertainty is more than acceptable given that the alternative coupling enables using grids of the order of millions of elements, profiting from much better description of heterogeneous reservoirs at a fraction of the calculation time of fully coupled models.
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