This study presents an extended numerical approach based on GeoMicro3D to simulate the reaction kinetics and three-dimensional (3D) microstructure evolution of alkali-activated fly ash (AAFA). Dissolution experiments were conducted under varying NaOH concentrations and temperatures to formulate predictive rate functions for Si and Al release. These experimentally derived kinetic functions, alongside a thermodynamic dataset for N-(C-)A-S-H gels, were incorporated into the GeoMicro3D model to capture the chemical reactions and 3D microstructure evolution of AAFA. The model well captured reaction degree of fly ash, formation of solid products, evolution of pore solution compositions, and porosity over time. Notably, it is the first to predict the time-dependent spatial distribution of phases within the 3D AAFA microstructure by integrating kinetic and microstructural modeling. Dual validation using both dissolution data and microstructural metrics demonstrates the model's reliability and robustness. This integrated framework provides new insights into the coupled chemical–microstructural evolution of alkali-activated materials.

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.