γ-Dicalcium silicate (γ-C2S) is known for its strong carbonation reactivity by which it can capture atmospheric carbon dioxide (CO2), thus, it can be used in construction industries. This paper aims to study the effects of γ-C2S on the properties of ground granulated blast-furnace slag (GGBFS) containing cement mortar and paste in natural and accelerated carbonation curing. The compressive strength of 5% γ-C2S (G5) added to GGBFS cement mortar is higher compared with the control one in natural carbonation (NC) and accelerated carbonation (AC) up to 14 days of curing, but once the curing duration is increased, there is no significant improvement with the compressive strength observed. The compressive strength of AC-cured mortar samples is higher than that of NC. The scanning electron microscopy (SEM) images show that the AC samples exhibited compact, uniform, and regular morphology with less in porosity than the NC samples. X-ray diffraction (XRD) and Fourier transform infra-red (FT-IR) results confirmed the formation of calcium carbonate (calcite: CC) as carbonated products in paste samples, which make the surface dense and a defect-free matrix result in the highest compressive strength. The decomposition of AC samples around 650–750 °C revealed the well-documented and stable crystalline CC peaks, as observed by thermogravimetry analysis (TGA). This study suggests that γ-C2S added to concrete can capture atmospheric CO2 (mostly generated from cement and metallurgy industries), and make the concrete dense and compact, resulting in improved compressive strength.
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