a b s t r a c tAmong the various risks associated with CO 2 storage in deep geologic formations, wells are important potential pathways for fluid leaks and groundwater contamination. Injection of CO 2 will perturb the storage reservoir and any wells that penetrate the CO 2 or pressure footprints are potential pathways for leakage of CO 2 and/or reservoir brine. Well leakage is of particular concern for regions with a long history of oil and gas exploration because they are top candidates for geologic CO 2 storage sites. This review explores in detail the ability of wells to retain their integrity against leakage with careful examination of the coupled physical and chemical processes involved. Understanding time-dependent leakage is complicated by the changes in fluid flow, solute transport, chemical reactions, and mechanical stresses over decade or longer time frames for site operations and monitoring.Almost all studies of the potential for well leakage have been laboratory based, as there are limited data on field-scale leakage. Laboratory experiments show that CO 2 and CO 2 -saturated brine still react with cement and casing when leakage occurs by diffusion only. The rate of degradation, however, is transport-limited and alteration of cement and casing properties is low. When a leakage path is already present due to cement shrinkage or fracturing, gaps along interfaces (e.g. casing/cement or cement/rock), or casing failures, chemical and mechanical alteration have the potential to decrease or increase leakage risks. Laboratory experiments and numerical simulations have shown that mineral precipitation or closure of strain-induced fractures can seal a leak pathway over time or conversely open pathways depending on flow-rate, chemistry, and the stress state. Experiments with steel/cement and cement/rock interfaces have indicated that protective mechanisms such as metal passivation, chemical alteration, mechanical deformation, and pore clogging can also help mitigate leakage. The specific rate and nature of alteration depend on the cement, brine, and injected fluid compositions. For example, the presence of co-injected gases (e.g. O 2 , H 2 S, and SO 2 ) and pozzolan amendments (fly ash) to cement influences the rate and the nature of cement reactions. A more complete understanding of the coupled physical-chemical mechanisms involved with sealing and opening of leakage pathways is needed.An important challenge is to take empirically based chemical, mechanical, and transport models reviewed here and assess leakage risk for carbon storage at the field scale. Field observations that accompany laboratory and modeling studies are critical to validating understanding of leakage risk. Long-term risk at the field scale is an area of active research made difficult by the large variability of material types (cement, geologic material, casing), field conditions (pressure, temperature, gradient in potential, residence time), and leaking fluid composition (CO 2 , co-injected gases, brine). Of particular interest are the circum...

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A numerical model was developed with the use of reactive transport code CrunchFlow to estimate porosity, permeability and mineral composition changes of Mount Simon sandstone under typical geological carbon sequestration conditions (P=23.8 MPa and T=85 o C). The model predicted a permeability decrease from 1.60 mD to 1.02 mD for the Mount Simon sandstone sample in a static batch reactor after 180 days of exposure to CO 2-saturated brine, which is consistent with measured permeability results. Model-predicted solution chemistry results were also consistent with laboratory-measured solution chemistry data. SiO 2 (am) was the primary mineral that causes permeability decrease, followed by kaolinite. Both SiO 2 (am) formation and kaolinite formation were attributed to the dissolution of quartz and feldspar. This study shows that the formation of SiO 2 (am) and kaolinite in the pore space of host rock is possible under typical CO 2 sequestration conditions. SiO 2 (am) and kaolinite precipitation at the CO 2 plume extent could reduce the permeability of host rock and improve lateral containment of free-phase CO 2 , contributing to overall security of CO 2 storage.

The implementation of acid gas cosequestration requires investigation of the potential for acid gas leakage along existing wellbores at sequestration sites. In this study, the interaction between pozzolan-amended wellbore cement (35 vol % pozzolan/65 vol % cement, hereafter referred to as 35:65 sample) and acid gas (e.g., a mixture of CO 2 and H 2 S) was simulated using the reactive transport code CrunchFlow. The model was applied to describe, interpret, and extrapolate scanning electron microscopy-backscattered electron (SEM-BSE) and scanning electron microscopy-energy dispersive spectroscopy (SEM-EDS) results on pozzolan-amended cement samples exposed to a 1 wt % NaCl solution saturated with an acid gas mixture of 21 mol % H 2 S and 79 mol % CO 2 under the temperature of 50 °C and pressure of 150 bar. Simulation outputs included calcite volume percentage, total Ca and S weight percentages in the solid phase, porosity, and effective permeability from the surface to the interior of pozzolan-amended wellbore cement. The model reproduced the observed calcite zone formed in the brine-cement interface region of the sample after 2.5 days of exposure. The model also predicted that the calcite layer became dense (calcite vol % in the layer reached 55%) after 90 days of exposure, consistent with the experimental observation. C−S−H was the primary Ca 2+ source to form the calcite layer, followed by C3S and Ca(OH) 2 . The main observed products of reaction between the 35:65 sample and H 2 S were pyrite and ettringite. Pyrite was primarily formed within 0.5 mm from the brine-cement interface; ettringite mainly formed within 1 mm from the interface. The model simulated these reactions that only the interface region (up to 2 mm distance from the surface) of the 35:65 sample became porous after 30 years of exposure. However, this narrow porous region could still serve as a migration pathway for acid gas, which was indicated by the increase in effective parallel permeability values determined from the simulation results. Those results show consistency with results of neat cement samples exposed under similar conditions. An increase in H 2 S content (in the range of 0 mol % to 40 mol %) results in more dissolution of Ca-bearing minerals in cement and more precipitation of calcite. Overall, this study indicates that an increase of porosity and permeability of pozzolan-amended wellbore cement at the cement interface with brine saturated with CO 2 and H 2 S can cause significant changes in effective permeability of the cement.

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