Influence mechanisms of CaCO3/NaAlO2 ratios in carbonaluminate cementitious materials

This study investigated the carbonaluminate cementitious materials (i.e., sodium aluminate (NaAlO2)-activated limestone pastes) with gradient calcite (CaCO3)/NaAlO2 molar ratios ranging from 1:1 to 6:1 (samples M1 to M6). NaAlO2 dosage affected the reaction process, hydration product, and cementitious property of the formed pastes. The thermonatrite (Na2CO3·H2O) and AH3 phase as hydration products exist in all the samples. Microcrystalline AH3 phase (crystallite size is near 22 nm) held a superior cementitious property, which was evidenced by diffraction spots scattered on concentric rings in transmission electron microscopy (TEM) results. Other hydrates varied with the CaCO3/NaAlO2 ratio. In case of lower CaCO3/NaAlO2 ratio (i.e., M1), NaAlO2 was incompletely consumed. The residual NaAlO2 promoted the formation of cubic-shaped katoite (3CaO·Al2O3·6H2O). Such hydrate barely contributed to the cementitious property of the formed matrix. When the CaCO3/NaAlO2 ratio reached 1.5:1 (e.g., M1.5-M6), NaAlO2 was entirely consumed, and monocarboaluminate (Mc, 3CaO·Al2O3·CaCO3·11H2O) instead of katoite was preferentially generated. The amounts of total hydrates decreased with the increasing CaCO3/NaAlO2 ratio, leading to the degraded properties of formed matrix. Thus, the 28-day compressive strength of M1.5 was the highest among these samples, reaching 35.55 MPa.