Relating chemical composition, structure, and rheology in alkali‐activated aluminosilicate gels.

Model aluminosilicate (N‐A‐S‐H) gel systems give insight to the complex reaction occurring in alkali‐activated binders, allowing for more precise control over chemical composition and exhibiting simpler kinetics. Small angle neutron scattering, oscillatory rheology, and solid‐state NMR were used to characterize N‐A‐S‐H gel samples and relate structure, chemical composition, and rheology. Aluminum concentration was varied in the gel samples at fixed silica and sodium concentration. Past the percolation point, the gel develops in two regimes distinct in structure and rheological behavior. The first gel regime is characterized by increase in modulus and initial formation of fractal structures following a diffusion‐limited monomer‐cluster aggregation mechanism. The second gel regime at higher aluminum concentrations is characterized by a modulus plateau and structure development via reaction‐limited aggregation of existing clusters. NMR data indicate a saturation of aluminum in the network at the transition between gel regimes, which may be pH driven. Understanding the structure‐property relationships critical to formation of the N‐A‐S‐H gel can give valuable insight to the reaction mechanism in alkali‐activated binders and the influence of chemical composition on resultant structure and mechanical properties. [ABSTRACT FROM AUTHOR]