AbstractSteel slag, a major industrial waste in China, possesses significant CO2 absorption potential. In this study, the CO2 sequestration of steel slag reached up to 15.6%; however, excessive mineralization resulted in reduced hydration activity. Compared to unmineralized slag, the 1‐day compressive strength decreased by 15.9%, and cumulative hydration heat over 72 h dropped by 8%. Using advanced visualization techniques such as scanning electron microscopy‐backscattered electron (SEM‐BSE), 3D X‐ray, and focused ion beam‐transmission electron microscopy (FIB‐TEM), the study reveals the microstructure of overmineralized steel slag, identifying a composition of a calcite outer layer, an amorphous SiO2 layer, a transition area, and an unmineralized core. The mineralization reaction affected 84.80% of the steel slag particles, with volume expansion causing dense regions to become porous, increasing porosity from 0% to 1.62%. This expansion also risks lattice distortion. During CO2 mineralization, a dense calcite layer forms, blocking the hydration of internal silicate gels and calcium silicate minerals, reducing the hydration activity of overmineralized slag. This study offers insights for optimizing CO2 mineralization techniques and applications for steel slag.
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