Green Cement Innovations: Use of Pillared Clays to Increase the Environmental Friendliness and Durability of Cement Materials

Cement production is associated with substantial carbon dioxide (CO₂) emissions due to the high material and energy intensity of Portland clinker manufacture. Partial clinker replacement with supplementary cementitious materials is one of the most promising strategies for reducing the carbon footprint of cement; however, the thermal activation of aluminosilicate raw materials does not always yield highly reactive products. In this study, a pillaring approach is proposed as a controlled method for modifying the structure of clays and unlocking their latent reactivity. Different clay types—namely, kaolinitic, montmorillonitic, and illite–chlorite clays—were sequentially treated with an aluminum sulfate solution and calcined at 650 °C. Their phase composition and microstructure were characterized by X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), and scanning electron microscopy (SEM), while specific surface area was determined by BET analysis and pozzolanic activity. The results showed that pillaring doubled the specific surface area of montmorillonitic (2:1) and illite–chlorite (2:1:1) clays. Replacing 30% of clinker with pillared clays and limestone increased the compressive strength to 86.5 MPa and the flexural strength to 34.6 MPa. The developed low-carbon composite cements also exhibited high durability: the density of the hardened cement mortar increased to 2.410 g/cm³, the strength loss after 200 freeze–thaw cycles decreased to ≤5.5%, and the sulfate resistance coefficient (Ks) increased to 0.98 (with minimal expansion of the samples <0.02%). The proposed approach makes it possible to reduce the carbon footprint of cement by 25–30% while enabling the use of locally available raw materials for the production of competitive low-carbon green cements. Reported reductions of this order are broadly consistent with the known effect of lowering clinker content through supplementary cementitious materials in blended cement systems.