Dissolution processes, hydrolysis and condensation reactions during geopolymer synthesis: Part I—Low Si/Al ratio systems

Abstract

Initial geopolymeric reaction processes governing dissolution of solid aluminosilicate particles in alkali solutions have been investigated using conventional experimental techniques, and the data analysed by speciation predictions of the partial charge model (PCM). For metakaolin powders activated with 5.0 M NaOH, solid-state nuclear magnetic resonance (NMR) spectra disclose the existence of monomeric [Al(OH)₄]⁻ species after two hours of dissolution, consistent with PCM predictions. However, no equivalent monomeric silicate species were observed for 5.0–10.0 M NaOH activator solutions characteristic of systems with nominal Si/Al ≤ 1. The apparent absence of monomeric silicate species suggest rapid condensation of silicate units with [Al(OH)₄]⁻ to generate aluminosilicate species, as indicated by the evolution of the shoulder at around −87 ppm in the ²⁹Si NMR spectra. Of the two possible stable silicate species [SiO₂(OH)₂]²⁻ and [SiO(OH)₃]⁻, the latter appears most likely to condense with [Al(OH)₄]⁻ to produce aluminosilicate oligomers, from which larger oligomers subsequently form through further condensation with [Al(OH)₄]⁻ leading to a gradual build up of aluminosilicate networks and a lowering of system alkalinity. This dissolution and hydrolysis sequence at the early stages of synthesis suggests a reaction path wholly consistent with predictions of the partial charge model.