The hydration and hardening of α-hemihydrate phosphogypsum (HH) prepared in the absence and presence of L-Aspartic acid (L-Asp) were investigated by thermodynamic analysis, measurements of ion concentrations and crystal water content, and morphology observation. In addition, computed tomography (CT) scanning was proposed to analyze the hole characteristic of hardened gypsum in situ. The results show that HH will pass through the unstable region and the stable region of dihydrate gypsum (DH) in turn during the hydration. The hydration of HH follows the dissolution–crystallization principle; the hydration process can be divided into the dissolution stage, dissolution–crystallization stage and equilibrium stage. Compared with the HH prepared without crystal modifier, the hydration process of HH prepared with L-Asp is obviously prolonged, and the morphology of DH changes from needle-like to diamond-shape crystals with an aspect ratio of 1:1. Meanwhile, the defect-specific surface and porosity of hardened gypsum significantly decreases, achieving a more compact, hardened paste with higher compressive strength.
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