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Abstract An effective method to make cement and concrete more sustainable is to blend them with the proper supplementary cementitious materials (SCMs). This study evaluates a pair of schist‐type materials with slightly different phase compositions, as a partial replacement for ordinary Portland cement (OPC). Materials received from several mines in ground powder form were studied by X‐ray diffraction, thermogravimetric analysis (TGA), and scanning electron microscopy. According to the TGA results, the activation procedures for the candidate SCMs were determined. The as‐received powders were heat treated in three different decomposition regimes (30%, 50%, and 80% of the total weight losses during thermal decomposition). These regimes corresponded to the activation level of the potential SCMs due to the de‐hydroxylation of the clay‐type minerals within them. Pozzolanic reactivity (pozzolanicity) of untreated as well as treated powders were estimated via electrical conductivity measurements in saturated calcium hydroxide solution. Blended cement pastes with 30 wt.% of OPC substituted with calcined clay‐type materials have developed mechanical properties equal to those of pure cement (100 wt.% OPC) paste after 28 days of hydration time. Two blended cement pastes prepared with candidate SCMs were compared to 100% OPC and OPC composite paste with metakaolin, which is regarded in the literature as a standard.

To develop a more reactive pozzolan for supplementary cementitious materials (SCMs), the co-calcination of kaolinite and limestone was investigated for its contribution to hydration of blended cement. Kaolinite (with ~50 wt% quartz impurity) was calcined at 700 °C, and a mixture of kaolinite and limestone was calcined at 800 °C. These activated SCMs were added to ordinary Portland cement (OPC), replacing ca. 30 wt% of the OPC. The compressive strength of these blended cement paste samples was measured after 28 and 90 days, while the hydration products and microstructural development in these blended cement pastes were analyzed by X-ray diffraction (XRD), thermogravimetric analysis (TGA), and scanning electron microscopy (SEM). The results revealed that adding free lime to OPC, together with metakaolin, led to enhanced compressive strength. The compressive strength of this new blended cement paste reached 113% and 112% of the compressed strength of pure OPC paste after 28 and 90 days of hydration, respectively. Furthermore, this study showed that the improvement was due to the increased consumption of Portlandite (CH), the formation of calcium aluminosilicate hydrate (CASH), and the reduction of porosity in the sample containing free lime and metakaolin.