On the interaction of pure and impure supercritical CO2 with rock forming minerals in saline aquifers: An experimental geochemical approach

Wilke, Franziska; Vásquez, Mónica; Wiersberg, Thomas; Naumann, Rudolf; Erzinger, J.

doi:10.1016/j.apgeochem.2012.04.012

Cited by 64 publications

(36 citation statements)

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“…However, the natural alkalinity of reservoir rock with the presence of trace to moderate carbonates may buffer the initially lowered pH, as has been observed for pure CO 2 injection into the Frio formation, USA (Kharaka et al, 2006). Pure calcite mineral separates and moderate calcite in sandstone core have been observed experimentally to buffer the acidity generated by co-injection of SO 2 with CO 2 to~pH 6 in two studies Wilke et al, 2012). SO 2 co-injection with CO 2 also has the potential for increased ferroan carbonate mineral dissolution to occur compared to pure CO 2 injection, and hence increased cation release into solution (and potentially reservoir porosity-permeability in the short term).…”

Section: Introductionmentioning

confidence: 87%

“…Injecting CO 2 containing SO 2 , O 2 and NO 2 has been predicted or observed to result in the formation of acids stronger than carbonic acid, e.g. sulfuric, and nitric acids (Wilke et al, 2012). Co-injection of impurities such as SO 2 has been predicted to reduce formation water pH to as low as 0-1 (Gunter et al, 2000;Knauss et al, 2005;Xu et al, 2007).…”

Section: Introductionmentioning

confidence: 97%

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SO2–CO2 and pure CO2 reactivity of ferroan carbonates at carbon storage conditions

et al. 2015

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Section: Introductionmentioning

confidence: 87%

Section: Introductionmentioning

confidence: 97%

SO2–CO2 and pure CO2 reactivity of ferroan carbonates at carbon storage conditions

et al. 2015

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“…Many investigations have put emphasis on the geochemical effects of the impurities contained in the CO 2 streams, including the brine acidification effects by co-injected SO 2 , NO 2 , or H 2 S and the corresponding effects on the porosity and permeability of reservoir and caprock, e.g. [10][11][12][13][14][15], and the hydrocarbon oxidation by the O 2 impurity, e.g. [16][17].…”

Section: Introductionmentioning

confidence: 99%

Numerical investigation of the partitioning phenomenon of carbon dioxide and multiple impurities in deep saline aquifers

Jiang

2017

Applied Energy

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Highlights• The partitioning behaviours of impure CO 2 in geological formations are investigated.• The effects of N 2 , CH 4 or the mixture of N 2 and CH 4 are generally similar.• Less soluble N 2 and CH 4 enhance gas breakthroughs and the partitioning.• More soluble species such as H 2 S dissolves preferentially in the formation brine. AbstractThe partitioning behaviours of CO 2 with three kinds of common impurities, i.e., N 2 , CH 4 and H 2 S, in the formation brine are investigated by numerical simulations. The results indicate that the effects of N 2 , CH 4 or the mixture of N 2 and CH 4 at the same concentrations are generally similar. The leading gas front is usually made up of less soluble impurities, such as N 2 , CH 4 or the mixture of N 2 and CH 4 , while more soluble species such as H 2 S has dissolved preferentially in the formation brine. The separations between different gas species increase as the gas displacement front migrates forwards and contacts more of the aqueous phase. Compared with the partitioning results of the 98% CO 2 and 2% H 2 S mixture, the results indicate that the inclusion of less soluble N 2 and/or CH 4 results in an earlier gas breakthrough and a longer delay between the breakthrough times of CO 2 and H 2 S. The early breakthrough of the gas phase is mainly because that the addition of N 2 and/or CH 4 lowers the viscosity of the gas phase, resulting in a higher gas velocity than that of the CO 2 -H 2 S mixture. Meanwhile, the mobility ratio is higher and the gas mixture contacts the formation brine over a larger area, giving rise to more efficient stripping of the more soluble gas species like H 2 S and thus larger separations. In the meantime, with the same total concentrations of impurities (12%), when 2% H 2 S is contained in the CO 2 streams, gas phase flows slower and thus the breakthrough time is later. Furthermore, the effects on the partitioning phenomenon are weaker with decreasing concentrations of N 2 and/or CH 4 (from 10% to 2%) with fixed concentrations of other impurity like H 2 S (2%). The migration distances and the separations between different gas species change linearly with time on the whole, as confirmed by a simulation in a longer model.

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“…During geologic carbon sequestration, oxidative dissolution of sulfide minerals in the reservoir rock or caprock can occur in the presence of dissolved oxygen (Evangelou and Zhang 1995;Lowson 1982;Moses et al 1987) and subsequently release toxic metals and radionuclides such as uranium into the brine (Keating et al 2010;Little and Jackson 2010). Although a number of previous experimental studies have focused on changes in the major ion composition and mineralogical alteration during the interaction between caprock and CO 2 -brine or supercritical CO 2 (Alemu et al 2011;Credoz et al 2009;Liu et al 2012;Wilke et al 2012), few studies have addressed the effects of redox processes on toxic contaminant mobilization due to other gases co-injected with CO 2 during geologic carbon sequestration. This study focuses on the effect of oxygen in the CO 2 stream on the mobilization of toxic contaminants (e.g., metals and radionuclides) from a caprock (Gothic shale from the Aneth Oil Field, Utah) during the interaction with CO 2 -brine under geological carbon sequestration conditions.…”

Section: Introductionmentioning

confidence: 99%

FY12 ARRA-NRAP Report ? Studies to Support Risk Assessment of Geologic Carbon Sequestration

Cantrell¹,

Shao²,

Thompson³

et al. 2011

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SummaryThis report summarizes results of research conducted during FY 2012 to support the assessment of environmental risks associated with geologic carbon dioxide (CO 2 ) sequestration and storage. Several research focus areas are ongoing as part of this project. This includes the quantification of the leachability of metals and organic compounds from representative CO 2 storage reservoir and caprock materials, the fate of metals and organic compounds after release, and the development of a method to measure pH in situ under supercritical CO 2 (scCO 2 ) conditions.Metal leachability experiments were completed on six different rock samples in brine in equilibrium with scCO 2 at representative geologic reservoir conditions. In general, the leaching of Resource Conservation and Recovery Act of 1976 metals and other metals of concern was found to be limited and not likely to be a significant issue (at least, for the rocks tested). Metals leaching experiments were also completed on one rock sample with scCO 2 containing oxygen at concentrations of 0%, 1%, 4%, and 8% to simulate injection of CO 2 originating from the oxy-fuel combustion process. Significant differences in the leaching behavior of certain metals were observed when oxygen is present in the CO 2 . These differences resulted from oxidation of sulfides, release of sulfate, ferric iron and other metals, and subsequent precipitation of iron oxides and some sulfates such as barite.Experiments to evaluate the potential for mobilization of organic compounds from representative reservoir materials and cap rock and their fate in porous media (quartz sand) have been conducted. Results with Fruitland coal and Gothic shale indicate that lighter organic compounds were more susceptible to mobilization by scCO 2 compared to heavier compounds. Alkanes demonstrated very low extractability by scCO 2 . No significant differences were observed between the extractability of organic compounds by dry or water saturated scCO 2 . Reaction equilibrium appears to have been reached by 96 hours.When the scCO 2 was released from the reactor, less than 60% of the injected lighter compounds (benzene, toluene) were transported through the dry sand column by the CO 2 , while more than 90% of the heavier organics were trapped in the sand column. For wet sand columns, most (80% to 100%) of the organic compounds injected into the sand column passed through, except for naphthalene which was substantially removed from the CO 2 within the column.A spectrophotometric method was developed to measure pH in brines in contact with scCO 2 . This method provides an alternative to fragile glass pH electrodes and thermodynamic modeling approaches for estimating pH. The method was tested in simulated reservoir fluids (CO 2 -NaCl-H 2 O) at different temperatures, pressures, and ionic strengths, and the results were compared with other experimental studies and geochemical models. Measured pH values were generally in agreement with the models, but inconsistencies were present between some of the models.v

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On the interaction of pure and impure supercritical CO2 with rock forming minerals in saline aquifers: An experimental geochemical approach

Cited by 64 publications

References 34 publications

SO2–CO2 and pure CO2 reactivity of ferroan carbonates at carbon storage conditions

SO2–CO2 and pure CO2 reactivity of ferroan carbonates at carbon storage conditions

Numerical investigation of the partitioning phenomenon of carbon dioxide and multiple impurities in deep saline aquifers

FY12 ARRA-NRAP Report ? Studies to Support Risk Assessment of Geologic Carbon Sequestration

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