Calcium
silicate minerals can react with CO2 to form
calcium carbonate and have been proposed to be a sustainable binder
as a potential CO2 sinker. In this study, the carbonation
characteristics are comparatively assessed among calcium silicates
having different calcium/silica (Ca/Si) ratios and polymorphs (CS,
C3S2, γ-C2S, β-C2S, C3S). Calcium silicate compacts exposed to a
100% CO2 environment at a 0.4 MPa pressure were tested
for carbonation temperature evolution, degree of carbonation (DOC),
mechanical properties, and microstructural characterization. Results
indicate γ-C2S is the most reactive, reaching a DOC
of 50% in 24 h, followed by C3S2, CS, β-C2S, and C3S, which generally agrees with the pattern
of the cumulative normalized temperature increase. Meanwhile, carbonated
β-C2S compact attains the highest compressive strength
of 80 MPa in 24 h, followed by γ-C2S, C3S2, and C3S, while CS only reaches 20 MPa.
Calcite and aragonite are the preferable polymorphs of calcium carbonate
in the carbonated C3S, γ-C2S, β-C2S, and C3S2, while only the carbonation
of CS generates vaterite in addition to calcite and aragonite. The
unreacted grains coated by a thin rim of calcium-modified silica gels
are encapsulated by the continuous calcium carbonates, which composes
the skeleton of the carbonated calcium silicates.