2D reactive transport modeling of the interaction between a marl and a CO2-rich sulfate solution under supercritical CO2 conditions

The circulation of CO2-rich solutions through fractured marl cores (caprock) under different flow rates and supercritical CO2 conditions (PTotal = 150 bar, pCO2 = 61 bar and T = 60 °C) led to mineral changes caused mainly by calcite dissolution and to a lesser extent by aluminosilicate dissolution,...

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Detalles Bibliográficos
Autores: Dávila Ordóñez, Maria Gabriela, Luquot, Linda, Soler Matamala, Josep M., Cama Robert, Jordi
Tipo de recurso: artículo
Fecha de publicación:2016
País:España
Institución:Universitat Politècnica de Catalunya (UPC)
Repositorio:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglés
OAI Identifier:oai:upcommons.upc.edu:2117/101922
Acceso en línea:https://hdl.handle.net/2117/101922
https://dx.doi.org/10.1016/j.ijggc.2016.08.033
Access Level:acceso abierto
Palabra clave:Geological carbon sequestration
CO2 sequestration
Numerical modeling
Leakage
Marl caprock
Calcite dissolution
Gypsum precipitation
Anhídrid carbònic -- Segrest
Àrees temàtiques de la UPC::Enginyeria civil::Geologia
Descripción
Sumario:The circulation of CO2-rich solutions through fractured marl cores (caprock) under different flow rates and supercritical CO2 conditions (PTotal = 150 bar, pCO2 = 61 bar and T = 60 °C) led to mineral changes caused mainly by calcite dissolution and to a lesser extent by aluminosilicate dissolution, and by gypsum precipitation adjacent to the fracture walls. Another significant result was the formation of the altered and highly porous zone (Dávila et al., 2016a). Dissolution structures ranged from face to uniform dissolution and wormhole formation depending mainly on the flow rate. 2D reactive transport models were used to interpret the results of the percolation experiments (except at 60 mL h-1). They reproduced the variation in the outflow composition with time and the observed width of the altered zone along the fractures. A good match was achieved by using initial Deff values in the rock matrix that ranged from 1 × 10-13 m2 s-1 to 3 × 10-13 m2 s-1 under slow flow rates. The Deff value was higher by a factor of 20 (6 × 10-12 m2 s-1) under fast flow. Moreover, a slight variation in the calcite reactive surface areas contributed to the fit of the model to the experimental data. The modeling results reproduced major dissolution of calcite and gypsum precipitation, and minor dissolution of clinochlore. Calcite dissolution was boosted by increasing the flow rate and gypsum precipitation increased at intermediate flow rate (1 mL h-1). Minor precipitation of dolomite, kaolinite, boehmite and three zeolites (mesolite, stilbite and smectite) along the altered zone occurred. The magnitude of these reactions was consistent with the measured increase in porosity over the altered zone.