Hydro-dynamically controlled alteration of fractured Portland cements flowed by CO2-rich brine

• We investigated the effect of CO2 rich-brine flowing through fractured Portland cements under in situ CO2 storage conditions.
• Carbonation process is dominant during CO2 low flow injection.
• During high flow rate injection, the permeability remains constant due to the precipitation of a secondary phase (Si-rich amorphous phases).

Deficient sealing in the well cement plugs and annulus due to mechanical fracturing is an important risk of CO2 leakage from the reservoir to others permeable layers and the surface. Such situation was reproduced at laboratory scale in order to determine the hydro-chemical control on the fracture permeability. Specifically, we investigated the effect of CO2 rich-brine flowing through fractured Portland cements at T = 60 °C and P = 10 MPa and variable flow rates. We showed that carbonation process is dominant and induces permeability decrease and leakage mitigation for extremely low flow rate whereas for high flow rate injection the permeability remains constant due to the precipitation of a low density secondary Si-rich phase which maintains the initial fracture aperture. At intermediate flow rate the hydraulic aperture can increase due to the densification of the material triggered by the net precipitation of low porosity calcite. These results emphasize that more complex behaviors than those considered from batch experiments may take place in the vicinity of flowing fractures. Specifically, the redissolution of the neoformed calcite as well as the development of amorphous phases, both controlled by the CO2-rich brine renewing rate in the fracture may prevent the healing fracture.