Phosphorus slags, abundant industrial by-products, hold significant potential for use as supplementary cementitious materials (SCM). To explore its application, phosphorus slags with varying contents of P₂O₅ were synthesized, and their network structure, dissolution behaviour, and hydration products in cementitious systems were investigated. The results showed that the pozzolanic reactivity initially decreased and then increased with increasing P₂O₅ content from 3.11 to 8.32 wt%. This behaviour was attributed to the competition between silicate network repolymerization and distortion of aluminium polyhedra. Furthermore, the incorporation of phosphorus increased the fractions of Al_V and Al_VI in the glass network, which promoted the incongruent dissolution of Al over Si. Thermodynamic simulation predicted the formation of hydroxyapatite, as the main phosphorus-containing hydration product, which was further confirmed by XRD and NMR results, although with low crystallinity. These findings suggested new perspectives on adopting phosphorus slag as a SCM in cement and concrete production.

Alkali and alkali earth metal ions are normally present in the gels of alkali-activated materials as well as blended PC-based materials. Previous studies have revealed that the leaching of these cations can trigger the change in gel structure and even the gel decomposition. However, the dissolution of cations was rarely known and the underlying mechanisms remained unclear. To address this issue, five calcium-(sodium, potassium-)aluminum-silicate hydrates (C-(N,K-)A-S-H gels) with different Ca/Si ratios (0.8–1.2) and Al/Si ratios (0.1–0.3) were synthesized to investigate the leaching behaviour of Ca, Na and K. For the first time, the dissolution free energies of Ca, Na and K in C-(N,K-)A-S-H gels were calculated using molecular dynamics simulations with the metadynamics method. Experimental results showed that Na showed the highest leaching ratio, followed by K and Ca, attributed to the lowest dissolution free energy of Na. The gel with a higher Ca/Si ratio or a lower Al/Si ratio showed higher charge positivity on the surface, resulting in reduced leaching of the three cations. Additionally, the presence of K was found to promote the dissolution of Na in gels.

Calcium sodium aluminosilicate hydrate C-(N-)A-S-H gels, formed through the alkali-activation of calcium silicate-based materials, may exhibit greater susceptibility to aqueous environments when compared to traditional C-(A-)S-H phases formed by hydration of blended Portland cements. This study investigates structural changes in synthesized C-(N-)A-S-H gels triggered by water immersion. Three gels have been examined, each with stoichiometrically controlled ratios of Ca/Si (0.8 and 1.2), Al/Si (0.1 and 0.3), and Na/Si (0.1, 0.2, and 0.3). The gel with a higher Ca/Si ratio demonstrated enhanced resistance to water leaching and only experienced marginal decalcification whereas the gels with lower Ca/Si ratios exhibited more pronounced effects including leaching losses of Si. Notably, all gels displayed rapid and substantial sodium leaching, contributing to an increased degree of polymerization for the aluminosilicate tetrahedra in the gels. A plausible mechanism for this change is that Na leaches out from the interlayer and Ca ions progressively take over the role of charge compensators in the interlayer of the C-(N-)A-S-H structure.

Due to the satisfactory property and high productivity, heat-cured concretes have been widely used in engineering practice. However, heat curing process also brings some drawbacks that are detrimental to the long-term property of this material. To address this issue, lightweight fine aggregate (LWFA) was employed to provide internal curing (IC) for a heat-cured mortar (HCM) blended with fly ash (FA). The influences of LWFA on the interior relative humidity of HCM and the reaction environment and behavior of FA were measured. It was found that IC of LWFA could mitigate the drop of interior humidity and enhance the reaction degrees of cement and FA. This contributed significantly to the microstructure densification of HCM, higher compressive strength and better resistance to chloride ion. The results indicate that LWFA benefits to enhancing the efficiency of FA in a heat curing system and the combination of LWFA and FA contribute to improving the long-term property of HCM.