Stabilization of metastable calcium carbonate polymorphs on the surface of recycled cement paste particles: A two-step carbonation approach without chemical additives

In this study, a two-step carbonation method is developed to control the formation of calcium carbonate (Cc) polymorphs on the surface of recycled hardened cement paste (RHCP) without the use of chemical additives. In the first step, RHCP undergoes semi-dry carbonation under controlled humidity conditions, followed by wet carbonation at various temperatures in the second step. The results show that vaterite and aragonite are stabilized during the wet carbonation process, forming primarily on the surface of RHCP particles. The stabilization of the metastable Cc phases is driven by the synergistic effect of existing Cc seeds in the RHCP and the reaction temperature. A temperature range of 9–48 °C promotes the formation of vaterite, while higher temperatures (60–90 °C) lead to its dissolution. The calcite seeds present in RHCP do not enhance the formation of vaterite and aragonite during wet carbonation. This method offers a potential practical approach for valorizing concrete waste while capturing CO₂ from the atmosphere.