Insights into silicate carbonation processes in water-bearing supercritical CO2 fluids (original) (raw)

2013, International Journal of Greenhouse Gas Control

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Abstract

Long-term geologic storage of carbon dioxide (CO2) is considered an integral part to moderating CO2 concentrations in the atmosphere and subsequently minimizing effects of global climate change. Although subsurface injection of CO2 is common place in certain industries, deployment at the scale required for emission reduction is unprecedented and therefore requires a high degree of predictability.

Reactivity of dolomite in water-saturated supercritical carbon dioxide: Significance for carbon capture and storage and for enhanced oil and gas recovery

Energy Conversion and Management, 2013

Carbon dioxide injection in porous reservoirs is the basis for carbon capture and storage, enhanced oil and gas recovery. Injected carbon dioxide is stored at multiple scales in porous media, from the pore-level as a residual phase to large scales as macroscopic accumulations by the injection site, under the caprock and at reservoir internal capillary pressure barriers. These carbon dioxide saturation zones create regions across which the full spectrum of mutual CO 2-H 2 O solubility may occur. Most studies assume that geochemical reaction is restricted to rocks and carbon dioxide-saturated formation waters, but this paradigm ignores injection of anhydrous carbon dioxide against brine and water-alternating-gas flooding for enhanced oil recovery. A series of laboratory experiments was performed to evaluate the reactivity of the common reservoir mineral dolomite with water-saturated supercritical carbon dioxide. Experiments were conducted at reservoir conditions (55 and 110°C, 25 MPa) and elevated temperature (220°C, 25 MPa) for approximately 96 and 164 h (4 and 7 days). Dolomite dissolves and new carbonate mineral precipitates by reaction with water-saturated supercritical carbon dioxide. Dolomite does not react with anhydrous supercritical carbon dioxide. Temperature and reaction time control the composition, morphology, and extent of formation of new carbonate minerals. Mineral dissolution and re-precipitation due to reaction with water-saturated carbon dioxide may affect the contact line between phases, the carbon dioxide contact angle, and the relative permeability and permeability distribution of the reservoir. These changes influence fundamental properties of hysteresis of drainage and imbibition cycles, rock wettability, and capillary pressure. The efficacy of physical carbon dioxide trapping mechanisms, integrity of caprock, and injectivity of a carbon dioxide storage reservoir as well as the injectivity and production rate of an enhanced oil recovery operation may be affected.

Geological Storage of Carbon Dioxide

Environmental and Engineering Geoscience, 2009

Carbon dioxide is the main compound identified as affecting the stability of the Earth's climate. A significant reduction in the volume of greenhouse gas emissions to the atmosphere is a key mechanism for mitigating against climate change. Geological storage of CO 2, or the injection and stabilization of large volumes of CO 2 in the subsurface in saline aquifers, existing hydrocarbon reservoirs or unmineable coal-seams, is one of the more technologically advanced options available. A number of studies have been carried out aimed at understanding the behaviour and long term fate of CO 2 when stored in geological formations.

Carbonate geochemistry and its role in geologic carbon storage

2021

Massive quantities of CO 2 need to be captured and stored to address the potential consequences of global warming. Geologic storage of CO 2 may be the only realistic option available to store the bulk of this CO 2 due to the required storage volumes. Geologic storage involves the injection of CO 2 into the subsurface. This injection will lead to the acidification of the formation fluids and provoke a large number of fluid-mineral reactions in the subsurface. Of these reactions, those among CO 2-rich fluids and carbonate minerals may be the most significant as these reactions are relatively rapid and have the potential to alter the integrity of caprocks and well bore cements. This review provides a detailed summary of field, laboratory and modeling results illuminating the potential impacts of the injection of large quantities of CO 2 into the subsurface as part of geologic storage efforts

Geological Storage of CO2: a State-Of-The-Art of Injection Processes and Technologies

Oil & Gas Science and Technology, 2005

-Stockage géologique du CO 2 : état de l'art des technologies d'injection-Dans cet article, les technologies de puits nécessaires à l'injection de CO 2 sont présentées ainsi que les mécanismes physico-chimiques provoqués par l'injection autour du puits :-Les matériaux utilisés pour le puits et les procédures d'abandon de puits doivent être choisis de façon à éviter toute fuite de CO 2 le long du puits et d'assurer la sécurité à long terme du stockage.-La zone autour du puits subit des mécanismes de dissolution/reprécipitation causés par l'injection de CO 2 , qui peuvent influer sur l'injectivité. Ces phénomènes dépendent fortement des caractéristiques du réservoir et requièrent aujourd'hui une étude théorique et expérimentale approfondie afin de contrôler l'injectivité des puits d'injection de CO 2 , élément clé car de grandes quantités de CO 2 devront être injectées.

The CarbFix Pilot Project - Storing carbon dioxide in basalt

2011

In situ mineral carbonation is facilitated by aqueous-phase chemical reactions with dissolved CO 2 . Evidence from the laboratory and the field shows that the limiting factors for in situ mineral carbonation are the dissolution rate of CO 2 into the aqueous phase and the release rate of divalent cations from basic silicate minerals. Up to now, pilot CO 2 storage projects and commercial operations have focused on the injection and storage of anthropogenic CO 2 as a supercritical phase in depleted oil and gas reservoirs or deep saline aquifers with limited potential for CO 2 mineralization. The CarbFix Pilot Project will test the feasibility of in situ mineral carbonation in basaltic rocks as a way to permanently and safely store CO 2 . The test includes the capture of CO 2 flue gas from the Hellisheidi geothermal power plant and the injection of 2200 tons of CO 2 per year, fully dissolved in water, at the CarbFix pilot injection site in SW Iceland. This paper describes the design of the CO 2 injection test and the novel approach for monitoring and verification of CO 2 mineralization in the subsurface by tagging the injected CO 2 with radiocarbon ( 14 C), and using SF 5 CF 3 and amidorhodamine G as conservative tracers to monitor the transport of the injected CO 2 charged water.

Supercritical CO 2 injection and residence time in fluid-saturated rocks: Evidence for calcite dissolution and effects on rock integrity

International Journal of Greenhouse Gas Control, 2017

CO 2 injection and storage in geological reservoirs is an attractive prospect for mitigating the anthropogenic production of greenhouse gases and global warming. The technology could lead to mineral precipitation and therefore stable storage over geological time scales. This contribution investigates the evolution of three calciterich reservoir rock analogues during injection of and exposure to supercritical CO 2 (scCO 2), i.e., two limestones (Tuffeau and Savonnieres) and a synthetic calcite-cemented sandstone (CIPS). Three types of exposure protocols have been conducted: (i) scCO 2 injection and a four-hour residence time in an initially dry rock; (ii) scCO 2 injection and a two-hour residence time in an initially brine-saturated rock; and (iii) scCO 2 injection and a fourhour residence time in an initially brine-saturated rock. Two aspects are monitored during these experiments: (i) the evolution of the pore fluid chemical composition; and (ii) the evolution of the rocks' physical properties (i.e. porosity, permeability, P-wave velocity and electrical resistivity). Additionally, some scCO 2 injection and exposure experiments in the brine-saturated rocks have been conducted using X-ray tomographic monitoring. X-ray tomographic monitoring suggests that scCO 2 first displaces the water, leading to an average water saturation of about 70-90%. Then, scCO 2 dissolves in the pore brine, leading to a homogeneous decrease by about 3% in water saturation of the sample. As a result, the pore brine acidifies even after 2 h of exposure only, which leads to calcite dissolution and a significant increase in the brine's concentration in calcium cations. For the samples and most exposure experiments, evidence of calcite dissolution is inferred from the measured physical properties. For the brine-saturated Tuffeau limestone and CIPS sandstone, calcite dissolution leads to significant mechanical weakening. For the brine-saturated Savonnieres limestone, the sample subject to twohour residence time shows evidence of calcite dissolution, whereas the sample after four-hour residence time does not. Calcite re-precipitation could be the cause of this unexpected response after four hours. − , CO 3 2−), a major component of carbonate rocks (e.g. CaCO 3

Natural geochemical analogues for carbon dioxide storage in deep geological porous reservoirs, a United Kingdom perspective

Oil & gas science and …, 2005

Analogues géochimiques naturels pour le stockage du dioxyde de carbone en réservoir géologique poreux profond : perspective pour le Royaume-Uni -La concentration élevée en CO 2 atmosphérique participe au réchauffement climatique. Une mesure d'atténuation consiste à capter le CO 2 émis par les centrales électriques qui utilisent des combustibles fossiles, et à le stocker dans des aquifères salins ou dans des gisements exploités d'hydrocarbures. Des projets de démonstration déjà en cours et des analyses techniques indiquent que cette mesure est viable. Le CO 2 doit rester confiné pendant au moins 10 000 ans pour que cette option technologique ait un impact climatique. En vue de fournir une évaluation solide des performances d'un site de stockage, à l'échelle de temps indiquée, une approche possible est d'étudier les accumulations naturelles de CO 2 . Celles-ci sont en particulier capables de donner des informations sur les interactions roche-CO 2 -saumure à des échelles de temps comprises entre le millier et la dizaine de millions d'années. Les champs de CO 2 naturel en mer du Nord (Brae, Miller, Magnus), situés à 4 000 m d'enfouissement et plus, ne montrent pas la néoformation des phases minérales souvent prédite par la modélisation géochimique. La calcite et les feldspaths peuvent constituer encore entre 5 et 20 % des minéraux de la roche, tandis que la dawsonite n'est pas observée. Il en est de même pour des exemples de réservoirs de grès situés dans le sud-est australien et en Arizona. Il est possible qu'un état de déséquilibre thermodynamique se soit maintenu, de sorte que les modèles existants ne sont pas capables de prédire correctement les évolutions minéralogiques réelles, sur les durées pertinentes pour la séquestration du CO 2 . Ces modèles nécessitent une meilleure calibration. Les données expérimentales, à l'échéance de quelques mois, ou celles déduites des situations de récupération assistée (CO 2 -EOR), à l'échéance de quelques dizaines années, sont en général trop courtes pour offrir toutes les calibrations nécessaires. En revanche, les analogues naturels peuvent aider à combler cette lacune. Le plateau du Colorado abrite un tel système naturel, où des gisements estimés à 100 Gm 3 de CO 2 ont pu s'accumuler, à partir de sources vocaniques d'âge inférieur à 5 Ma.

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Dissolved CO2 Injection to Eliminate the Risk of CO2 Leakage in Geologic Carbon Storage

Springer eBooks, 2018

Geologic carbon storage is usually viewed as injecting, or rather as storing, CO2 in supercritical phase. This view is very demanding on the caprock, which must display: (1) high entry pressure to prevent an upward escape of CO2 due to density effects; (2) low permeability to minimize the upwards displacement of the brine induced by the injected CO2; and (3) high strength to ensure that the fluid pressure buildup does not lead to caprock failure. We analyze the possibility of injecting dissolved CO2 and, possibly, other soluble gases for cases when the above requirements are not met. The approach consists of extracting saline water from one portion of the aquifer, reinjecting it in another portion of the aquifer and dissolving CO2 downhole. Mixing at depth reduces the pressure required for brine and CO2 injection at the surface. We find that dissolved CO2 injection is feasible and eliminates the risk of CO2 leakage because brine with dissolved CO2 is denser than brine without dissolved CO2 and thus, it sinks towards the bottom of the saline aquifer.

Limiting the risk inherent to geological CO 2 storage: The importance of predicting inorganic and organic chemical species behavior under supercritical CO 2 fluid conditions

Greenhouse Gases: Science and Technology, 2014

Field tests have clearly demonstrated that injecting CO 2 in geological storage sites results in the release of heavy metals and organic species to groundwater, implying that CO 2 injection may have potentially dramatic consequences for the environment. Numerous laboratory experiments using rock and cement samples from different geological formations typical of injection sites show that rocks reacting with synthetic or natural fl uids and supercritical CO 2 at their respective temperature and pressure conditions generate fl uids with As, Cr, Cu, Cd, Pb, Fe, and Mn concentrations above Environmental Protection Agency drinking water standards. The solubility of a compound in supercritical-CO 2 (sc-CO 2 ), expressed in terms of the compound's activity or fugacity, also depends on the composition of the phases present at the pressure and temperature of the storage site. In a brine sc-CO 2 system, estimating the activity of an inorganic compound or the fugacity of an organic compound is a prerequisite to predicting the solubility of a compound in sc-CO 2 phases. Available models (e.g. Pitzer equations) require the use of binary salt concentrations and are best applicable to polar ionic compounds; but the effect of brines on larger hydrocarbons has not yet been explored. New experimental data will be needed to determine the magnitude of pH effects on the partitioning behavior of organic acids and trace metal complexes from brine to sc-CO 2 .

Significance of carbonate buffers in natural waters reacting with supercritical CO 2 : Implications for monitoring, measuring and verification (MMV) of geologic carbon sequestration

Geophysical Research Letters, 2008

1] Successful geologic sequestration of carbon in deep saline aquifers requires accurate predictive models of rock-brine-CO 2 interaction. Often overlooked in siliciclastichosted saline reservoirs is the carbonate buffering of the groundwater. Carbonate minerals are ubiquitous, even in siliciclastic host rocks, resulting in some carbonate buffering. Geochemical modeling of rock-brine-CO 2 systems often do not accurately predict the geochemical evolution of the system leading to significant doubts in predicting the performance of carbon repositories. New data from a simple NaCl brine-plagioclase hydrothermal experiment tests carbon sequestration in dawsonite and sensitivity to carbonate buffering. This is contrasted to a NaCl brinesiliciclastic rock system containing some initial bicarbonate buffering, analogous to most saline-aquifer sequestration targets, and show that critical errors are caused by incomplete or inaccurate characterization of the in situ geochemistry. We provide a methodology that accurately predicts the in situ condition using samples collected from brine-rock-CO 2 experiments or well-heads in a carbon sequestration monitoring scenario. Citation: Newell, D. L., J. P. Kaszuba, H. S. Viswanathan, R. J. Pawar, and T. Carpenter (2008), Significance of carbonate buffers in natural waters reacting with supercritical CO 2 : Implications for monitoring, measuring and verification (MMV) of geologic carbon sequestration, Geophys. Res. Lett., 35, L23403,

Experimental characterization of nonwetting phase trapping and implications for geologic CO2 sequestration

International Journal of Greenhouse Gas Control

Geological carbon sequestration is being considered worldwide as a means of mitigating anthropogenic emission of greenhouse gases. During sequestration, carbon dioxide (CO 2) gas effluent is captured from coal-fired power plants or other concentrated emission sources and injected into saline aquifers or depleted oil reservoirs for long term storage. In an effort to fully understand and optimize CO 2 trapping efficiency, the capillary mechanisms that immobilize subsurface CO 2 were analyzed at the pore-scale. Pairs of proxy fluids representing the potential range of in-situ conditions of supercritical CO 2 (nonwet-ting fluid) and brine (wetting fluid) were used during experimentation. The two fluids were imbibed and drained from a flow cell apparatus containing a sintered glass bead core. Fluid parameters (such as interfacial tension and fluid viscosities) and flow rate were altered to characterize their relative impact on capillary trapping. Computed x-ray microtomography (microCT) ...

Geochemical Aspects of Geologic Carbon Storage

Applied Geochemistry, 2013

Geochemical Aspects of Geologic Carbon Storage Editors' introduction Carbon capture and storage (CCS) is a critical technology for reducing greenhouse gas (GHG) emissions to meet global emissions targets set for the year 2050 (IEA, 2012). In CCS, CO 2 produced from stationary sources (i.e. power plants, cement-and iron-producing facilities, and refineries) is diverted from the atmosphere via capture and subsequent injection into deep, stable geological formations for long term storage (i.e. geologic carbon storage). A rapid deployment of CCS is required to meet 2050 climate goals, but currently, implementation of CCS is behind target. Economic, political and regulatory drivers, in addition to public understanding and acceptance of CCS, must converge quickly to support the development of CCS technology. Understanding the science of geologic carbon storage affects drivers for CCS in a multitude of ways that include providing information relevant to: site selection, capacity estimation, injectivity, storage permanence, risk assessment, environmental impacts, monitoring, attribution, leakage quantification, regulatory guidelines, and incident response protocols (e.g. Dixon et al., 2012). The purpose of this special issue of Applied Geochemistry on Geochemical Aspects of Geologic Carbon Storage is to synthesize and present a selection of the most innovative and relevant geochemical research in this rapidly evolving field to support the path forward. It is anticipated that a compilation of important thinking and work in this area will be a useful tool as geologic carbon storage advances towards industrial implementation on a global scale. This special issue highlights how researchers are integrating a number of approaches to address the many geochemical unknowns associated with geologic carbon storage. These unknowns arise from the complexities and heterogeneities inherent in and among the different types of geologic systems being considered for CCS, which affect the systems' responses to CO 2 injection. Even though careful site selection for CO 2 repositories ensures little chance for CO 2 leakage, every potential scenario must be investigated and CO 2 fate and transport assessed at every scale from pore to basin and at every depth from the reservoir to atmosphere. These assessments must then be integrated to form best practice guidelines for CCS implementation. Over the last years, government and industry-funded deep injection pilot projects and shallow controlled releases have helped to identify and quantify physical and chemical processes, to develop numerical simulation models to explain the behavior of CO 2 in the subsurface, and to test monitoring methods. Researchers are increasingly integrating laboratory-based and field-based geochemical observation of natural and engineered systems with numerical simulation models to better understand how geological systems will react to large-scale CO 2 input over the long-term. The contributions in this special issue are