Toward Carbon-Negative Construction Materials: CO₂-Storing Alkali-Activated Waste-Based Binder

This study examines the carbonation behavior and CO₂ storage potential of a Ca-rich alkali-activated binder produced entirely from industrial residues, namely ladle furnace slag (LFS), coal ash (CA), and cement kiln dust (CKD). The system was designed as a one-part alkali-activated material (AAM), with CKD acting as an internal activator, and subjected to ambient curing, water curing, and accelerated CO₂ curing at ambient pressure. Phase evolution, microstructural development, and pore-structure characteristics were investigated using X-ray diffraction, FTIR spectroscopy, DSC–TG analysis, scanning electron microscopy, and X-ray micro-computed tomography, together with measurements of density, water absorption, and compressive strength. CO₂ curing fundamentally altered the reaction pathway of the binder, shifting it from hydration-dominated to carbonation-controlled phase evolution, leading to the decomposition of calcium-bearing hydrates and complete carbonation of non-hydraulic γ-belite with the formation of vaterite, aragonite, and calcite. These transformations induced pronounced microstructural densification, reflected in a near-doubling of compressive strength (>48 MPa), increased apparent density, reduced water absorption, and simplified pore-network topology. The results demonstrate that controlled carbonation is an effective post-treatment strategy for waste-derived alkali-activated binders, enabling simultaneous performance enhancement and permanent CO₂ sequestration.