Exploring the potential of stable isotope methods for identifying the origin of CO2 in the carbonation process of cementitious materials within the carbon capture and storage environment

Abstract

This study investigates the potential of stable isotope (δ13C) methods for exploring the carbonation process of cementitious materials, including well cement paste, portlandite (CH), and calcium silicate hydrate (C–S–H). Through comprehensive chemical and isotopic characterization, along with extensive data analysis, several key conclusions emerge. Firstly, the pH of the solution, as well as the solubility and pH characteristics of mineral phases (CH and C–S–H), are identified as influential factors impacting the kinetics, thermodynamics, and distribution of carbon isotopes (12C and 13C) during the reaction process. Secondly, the study uncovered that higher final pH values correlated with a DIC pool enriched with 13C and a higher εDIC-CO2 isotopic enrichment factor (10.7–12.6 ‰). Furthermore, higher levels of DIC content, solution electrical conductivity, and lower pH lead to higher δ13C–CaCO3 and greater εCaCO3-DIC isotope fractionation (−12.9 to −7.5 ‰). These conditions favor the formation of carbonate minerals with higher isotopic signature (δ13C–CaCO3), thus better preserving the δ13C-DIC isotope ratio. It was identified that the carbonate mineral (δ13C–CaCO3) formed through the carbonation of cementitious materials (class G cement, CH, and C–S–H) appears to preserve the isotopic signature of the δ13C–CO2 source. In conclusion, stable isotope methods could be a valuable tool for assessing and monitoring the cement carbonation process in Carbon Capture and Storage (CCS) wells, particularly when it is crucial to distinguish between injected and endogenous CO2.