In this study, the carbonation kinetics, phase development, and microstructure evolution of ternesite (C5S2$) phase were investigated via wet carbonation. The results indicated that ternesite exhibited remarkable carbonation reactivity, achieving approximately 95% completion of the carbonation reaction within 15 min and facilitating CO2 sequestration exceeding 340 g per kilogram of ternesite. The main carbonation products identified were aragonite, calcite, gypsum, and silica gel (Si-gel). The carbonation kinetics conformed to the surface coverage model, with the reaction proceeding through distinct stages of acceleration, deceleration, and stabilization, ultimately resulting in the formation of a “core-shell” structure. Notably, the crystalline phase of calcium carbonate (CC) underwent spontaneous transformation during the carbonation of ternesite. It is observed that CC exhibited a polycrystalline structure and underwent a distinct phase transformation from calcite to aragonite. The resulting CC was predominantly metastable, exhibiting low crystallinity and reduced crystallite size. These characteristics are attributed to the intrinsic properties of ternesite, particularly the presence of SO42− ions, which promote the formation and stabilization of metastable aragonite. Furthermore, the changes in crystalline and morphology of CC, induced by dissolution and re-precipitation process, disrupted the CC layer and thereby facilitated the release of another significant product, Si-gel. These distinctive carbonation behaviors suggest that ternesite has potential for broader applications, including its use as a supplementary cementitious material or as a precursor for the synthesis of high value-added products such as aragonite whiskers and nano-sized SiO2.
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