Binghuan Gao

Geopolymers exhibit broad application prospects, including construction and radiation shielding, which require excellent mechanical performances. However, investigations on the nature of geopolymerization reactions and their consequential impact on mechanical performance are still vague. In this study, the effect of the major factors of Si/Al ratio and curing time on the geopolymerization reaction and flexural strength were studied based on the microstructure evolution and chemical bonding formation analyzed using the SEM, FTIR, peak deconvolution, and XRD methods. The microstructure of geopolymers was transferred from initially layered smooth particles of kaolinite to a 3D network porous structure, corresponding to sodalite. A spectrum exclusive to the geopolymer structure occurred at 973 cm⁻¹, corresponding to the sodium aluminum silicate hydrate (N-A-S-H) links, the integral area of which represents the degree of geopolymerization reaction. Furthermore, a controllable reaction degree was achieved by adjusting the Si/Al ratio and curing time, where the maximum reaction degree of 55% was achieved at a Si/Al ratio of 1.94 when cured for 7 d. The correlation between the flexural strength and reaction degree was found to follow a proportional relationship, achieving a flexural strength of 21.11 MPa with a degree of 45%. This study provides insight into the development of mechanical strength through controlling the reaction process.

Geopolymer ceramics undergo a series of thermal phase transitions, progressing from an amorphous geopolymer gel to a crystalline phase, and eventually to an amorphous glass phase as the temperature increases. However, there is a lack of mechanism understanding regarding to the crystallization process and the subsequent thermal degradation. Here, we fundamentally investigated the kinetics of nepheline formation in Na‐based geopolymer systems and its thermal stability up to 1400°C. Nepheline crystallization is controlled by bulk nucleation and three‐dimensional crystal growth based on the Avrami factor of 4.64, where the activation energy of nepheline formation is 350.59 kJ/mol. High thermal stability of geopolymer ceramics is achieved due to the appearance of nepheline up to 1400°C with the Si/Al ratio ranging from 1.40 to 1.94, while melting and amorphous structure are formed above a higher Si/Al ratio of 2.22. The nature of sintering for geopolymer ceramics consists of shrinkage, expansion and shrinkage corresponding to dehydroxylation, crystallization, and densification, leading to a thermal shrinkage of 21% at 1400°C.