Influence of Gypsum Type on Early Hydration Kinetics and Autogenous Shrinkage of Supersulfated Cement-Based UHPC Matrix

Ultra-high-performance concrete (UHPC) matrix faces critical challenges of high carbon footprint and significant autogenous shrinkage. Supersulfated cement (SSC), a potentially lower-carbon binder comprising ground granulated blast-furnace slag and gypsum, offers a promising alternative. This study systematically investigated the effect of gypsum type—phosphogypsum (PG), dihydrate gypsum (DH), and anhydrite (AH)—on the early hydration and shrinkage behavior of UHPC matrix incorporating 30% SSC as Portland cement replacement. A multi-technique approach, including mechanical testing, isothermal calorimetry, XRD, TG-DSC, SEM, LF-NMR, and autogenous shrinkage measurements, was employed. Results demonstrate that gypsum type critically governs sulfate dissolution kinetics, thereby dictating phase assemblage and microstructural evolution. DH provides relatively rapid sulfate dissolution, promoting earlier AFt and gel formation, which is associated with the highest early strengths and a marked reduction in autogenous shrinkage. AH shows a slower but sustained sulfate supply, resulting in comparable 28-day strength with moderate shrinkage reduction. PG yielded the lowest autogenous shrinkage (374 μm/m at 7 d), but it also suffered from severe early-age retardation due to soluble phosphate impurities, as evidenced by the delayed hydration peak and lowest 3 d strength. This behavior is mainly related to strong early-age retardation, delayed hydration, delayed setting, and a prolonged low-stiffness state. These findings suggest that appropriate gypsum selection in SSC enables tailored early-age performance and improved volume stability in the UHPC matrix, offering guidance for utilizing industrial by-products such as phosphogypsum in sustainable high-performance concrete design.