Influence of Polycarboxylate Superplasticizer on Rheological Behavior and Early Interfacial Evolution of Phosphogypsum-Based Supersulfated Cement

Driven by global carbon reduction targets, supersulfated cement has emerged as a promising low-carbon cementitious material. This study investigates the influence of a polycarboxylate superplasticizer (PCE) on the rheological behavior and early interfacial evolution of phosphogypsum-based supersulfated cement (PSSC). Rheological measurements, pore solution ion analysis, hydration heat analysis, X-ray diffraction (XRD), and scanning electron microscopy coupled with energy-dispersive spectroscopy (SEM–EDS) are employed to correlate early hydration processes with structural development. The results indicate that the incorporation of PCE significantly reduces the initial yield stress and moderates the structural build-up rate. At a PCE dosage of 0.3 wt.%, the initial static yield stress decreases from 1313 Pa to approximately 125 Pa, while the structural build-up index Is,s reaches 10.19, indicating improved particle dispersion while maintaining progressive structural reconstruction during hydration. Phosphogypsum (PG) functions not only as a sulfate source but also as an active interfacial substrate that promotes the preferential nucleation of AFt on its surface. In the absence of PCE, continuous Ca–P-enriched layers form on PG particles, accompanied by localized AFt accumulation. After the incorporation of PCE, the primary crystalline phases remain unchanged; however, gypsum dissolution and AFt formation are delayed. Meanwhile, Ca–P enrichment shifts from continuous coverage to a more dispersed distribution, promoting the spatially separated growth of AFt crystals rather than dense localized aggregation. Overall, PCE influences the evolution of the structure and properties of the system by regulating early interfacial reactions and the spatial organization of hydration products.