PNNL

Abstract

Cement samples were reacted with CO2-saturated groundwater, with or without added H2S (1 wt.%), at 50°C and 10 MPa for up to 13 months (CO2 only) or for up to 3.5 months (CO2 + H2S) under static conditions. After the reaction, X-ray computed tomography images revealed that calcium carbonate precipitation (CaCO3) occurred extensively within the fractures in the cement matrix, but only partially along fractures at the cement-basalt interface. Exposure of a fractured cement sample to CO2-saturated groundwater (50°C and 10 MPa) over a period of 13 months demonstrated progressive healing of cement fractures by CaCO3(s) precipitation. After reaction with CO2 + H2S-saturated groundwater, CaCO3 (s) precipitation also occurred more extensively within the cement fracture than along the cement-basalt caprock interfaces. X-ray diffraction analysis showed that major cement carbonation products of the CO2 + H2S-saturated groundwater were calcite, aragonite, and vaterite, all consistent with cement carbonation by CO2-saturated groundwater. While pyrite is thermodynamically favored to form, due to the low H2S concentration it was not identified by XRD in this study. The cement alteration rate into neat Portland cement columns by CO2-saturated groundwater was similar at ~0.02 mm/d, regardless of the cement-curing pressure and temperature (P-T) conditions, or the presence of H2S in the brine. The experimental results imply that the wellbore cement with fractures is likely to be healed during exposure to CO2- or CO2 + H2S-saturated groundwater, whereas fractures along the cement-caprock interface are likely to remain open and vulnerable to the leakage of CO2