The synthesis of N-A-S-H gel with high Si/Al ratios (>2) has been rarely reported in the literature, leaving the establishment of a reliable synthesis route as an open challenge. This paper aims to synthesize N-A-S-H gels with Si/Al ratios ranging from 1 to 3 and establish their thermodynamic database. The effects of reaction temperature, reaction time, initial Si/Al, concentration of reactants and pH of the matrix on the Si/Al ratios of the synthesized N-A-S-H gel were investigated. Results showed that N-A-S-H gels with target Si/Al ratios can be synthesized by controlling the concentration of reactants, pH and initial Si/Al ratios. The solubility products of the obtained N-A-S-H gels were determined via dissolution tests at different temperatures, to determine thermodynamic data. The development of this experimentally derived thermodynamic database of N-A-S-H gels constitutes a crucial step in the advancement of thermodynamic modeling of geopolymer, providing valuable insight into geopolymer reactions and phase assemblages.

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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.

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Recycling aluminosilicate-based solid wastes is imperative to realize the sustainable development of constructions. By using alkali activation technology, aluminosilicate-based solid wastes, such as furnace slag, fly ash, red mud, and most of the bio-ashes, can be turned into alternative binder materials to Portland cement to reduce the carbon footprint of the construction and maintenance activities of concrete structures. In this paper, the chemistry involved in the formation of alkali-activated materials (AAMs) and the influential factors of their properties are briefly reviewed. The commonly used methods, including X-ray diffraction (XRD), scanning electron microscopy (SEM), thermogravimetric analysis (TG), nuclear magnetic resonance spectroscopy (NMR), and X-ray pair distribution function technology, to characterize the microstructure of AAMs are introduced. Typical characterization results of AAMs are shown and the limitations of each method are discussed. The main challenges, such as shrinkage, creep, efflorescence, carbonation, alkali–silica reaction, and chloride ingress, to conquer for a wider application of AAMs are reviewed. It is shown that several performances of AAMs under certain circumstances seem to be less satisfactory than traditional portland cement systems. Existing strategies to improve these performances are reviewed, and recommendations for future studies are given.@en