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This paper presents numerical simulations of reactive transport which may be induced in the caprock of an on-shore depleted gas reservoir by the geological sequestration of carbon dioxide. The objective is to verify that CO 2 geological disposal activities currently being planned for the study area are safe and do not induce any undesired environmental impact.In our model, fluid flow and mineral alteration are induced in the caprock by penetration of high CO 2 concentrations from the underlying reservoir, where it was assumed that large amounts of CO 2 have already been injected at depth. The main focus is on the potential effect of precipitation and dissolution processes on the sealing efficiency of caprock formations.Concerns that some leakage may occur in the investigated system arise because the seal is made up of potentially highly-reactive rocks, consisting of carbonate-rich shales (calcite+dolomite averaging up to more than 30% of solid volume fraction). Batch simulations and multi-dimensional 1D and 2D modeling have been used to investigate multicomponent geochemical processes. Numerical simulations account for fracture-matrix interactions, gas 2 phase participation in multiphase fluid flow and geochemical reactions, and kinetics of fluidrock interactions.The geochemical processes and parameters to which the occurrence of high CO 2 concentrations are most sensitive are investigated by conceptualizing different mass transport mechanisms (i.e. diffusion and mixed advection+diffusion). The most relevant mineralogical transformations occurring in the caprock are described, and the feedback of these geochemical processes on physical properties such as porosity is examined to evaluate how the sealing capacity of the caprock could evolve in time.The simulations demonstrate that the occurrence of some gas leakage from the reservoir may have a strong influence on the geochemical evolution of the caprock. In fact, when a free CO 2 -dominated phase migrates into the caprock through fractures, or through zones with high initial porosity possibly acting as preferential flow paths for reservoir fluids, low pH values are predicted, accompanied by significant calcite dissolution and porosity enhancement. In contrast, when fluid-rock interactions occur under fully liquid-saturated conditions and a diffusion-controlled regime, pH will be buffered at higher values, and some calcite precipitation is predicted which leads to further sealing of the storage reservoir.

. Predicting long-term geochemical alteration of wellbore cement in a generic geological CO2 confinement site: tackling a difficult reactive transport modeling challenge. Journal of Hydrology, Elsevier, 2012, 420-421, pp.340-359.

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Dolomitization of a carbonate platform can occur at different times and in different diagenetic environments, from synsedimentary to deep burial settings. Numerical simulations are valuable tools to test and select the model that, among different hypotheses compatible with field and geochemical data, best honour mass balance, kinetic and thermodynamic constraints. Moreover, the simulation can predict the distribution of the dolomitized bodies in the subsurface and evaluate porosity changes; valuable information for the oil industry. This study is the first attempt to reproduce and investigate the compaction dolomitization model. The diagenetic study of the Jurassic carbonate basin and palaeohigh system of the Po Plain indicates that the carbonates of the palaeohighs were dolomitized by basin compaction fluids. The main goal of the simulations is to evaluate the origin and evolution of the dolomitizing fluids and to provide insights regarding the distribution of the potential reservoir-dolomitized bodies in the Po Plain. The modelling process is subdivided into two steps: basin modelling and reactive transport modelling. The SEBE3 basin simulator (Eni proprietary) was used to create a three-dimensional model of the compacting system. The results include compaction fluid flow rate from the basin to the palaeohigh, compaction duration and a determination of the total amount of fluid introduced into the palaeohigh. These data are then used to perform reactive transport modelling with the TOUGHREACT code. Sensitivities on dolomite kinetic parameters suggest that dolomitization was an efficient process even at low temperatures, with differences mainly related to the dynamics of the process. Fluid composition is one of the main constraints, the sea water derived compaction fluid is proven to be efficient for dolomitization due to its relatively high Mg content. Simulations also confirmed that permeability is the most important factor influencing fluid flow and, consequently, the dolomite distribution in the formation. Permeable fractured zones have a strong influence, diverting the dolomitizing fluids from their normal path towards overlying or lateral zones. Moreover, the simulations showed that, after dolomite replacement is complete, the dolomitizing fluids can precipitate dolomite cement, causing over-dolomitization, with related localized plugging effects in the zone of influx. Mass balance calculations indicate that in the dolomitization compaction model, the amount of compaction water fluxed from the basin to the carbonate is the main constraint on dolomitization efficiency. This observation implies that the ratio between the volume of the basin undergoing compaction 209 and the volume of the palaeohigh is a limiting factor on the final size of the dolomitized bodies. An isolated palaeohigh could be an ideal site for pervasive replacement dolomitization due to the large volume of compaction fluids available compared with the carbonate rock volume. In the case of large platforms, the more permeable margin lithofac...

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This study characterizes the effects of fluid migration into a predominantly shale cover which seals the active geothermal system of Mt. Amiata (Tuscany, Italy). During Alpine orogenesis the shale unit was affected by regional metamorphism at the limit of the diagenesis-anchizone. Subsequently, the phyllosilicate clay minerals of the shales underwent significant alteration at diagenetic temperatures (175±25ºC as determined by the geochemical model) by the pervasive circulation of fluids activated by the geothermal field. The overall mineralogical assemblages indicate that the main transformations consisted mostly of destabilization of illite and formation of kaolinite together with large amounts of I-S mixed layers, with higher smectite content and decreased Reichweite I-S ordering (from R3 to R1) with respect to the original, unaltered phases. Application of computer modelling indicates that the circulation of CO2-rich geothermal fluids into the shale unit was responsible for the observed phyllosilicate clay mineral transformations.