Role of soluble aluminum species in the activating solution for synthesis of silico-aluminophosphate geopolymers

An aluminosilicate precursor, such as metakaolin, can be transformed into a cement-like geopolymer binder via a phosphate activation approach. This paper identifies the effect of the addition of aluminum species into the phosphate activating solution on the formation of such geopolymers, from the fresh to the hardened state. Activating solutions with Al/P molar ratios of 0, 0.1, and 0.3 were prepared by blending monoaluminum phosphate (MAP) and orthophosphoric acid (OPA). The rheological properties, fluidity, and setting times of the fresh geopolymer pastes and the compressive strength of the hardened geopolymer matrices were studied. Liquid-state Al-27 and P-31 nuclear magnetic resonance (NMR) measurements for the chemical environments of Al and P, and spectroscopic, thermal, and microscopic analyses revealed that the soluble aluminum in the phosphate activating solution played an important role during the geopolymerization process. Seeding of aluminum species through inclusion in the activating solution allowed a rapid sol/gel transition that improved the rheological properties and setting time of the fresh geopolymer pastes at ambient temperature. However, although the increased concentration of aluminum phosphate oligomers promoted by the soluble aluminum addition contributed to the formation of a compact matrix with high early strength, it hinders the ongoing reaction of metakaolin in the later period, which has a detrimental influence on ongoing strength development beyond 7 days of curing.