In this study, geopolymers were prepared using ladle furnace slag (LFS) and fly ash (FA), and hydrothermal treatment was then used to synthesize bulk zeolite molecular sieves with gismondine, zeolite-P1, and sodalite phases. The effect of the synthesis conditions on the crystalline phases of the zeolite molecular sieves was investigated by XRD. The results showed that the best zeolite molecular sieves were prepared with an LFS: FA ratio of 4: 6, a curing temperature of 40 °C, a curing time of 12 h, a sodium silicate modulus (Ms) of 1.4, a NaOH concentration of 4 mol/L, a hydrothermal temperature of 120 °C, and a hydrothermal time of 12 h. On this basis, the products were analyzed by SEM, N2 adsorption, and FT-IR. The results showed that the synthesized zeolite molecular sieves had mesoporous properties, and the degree of polymerization and cross-linking of the silica-aluminate gel were enhanced after hydrothermal treatment. In addition, the formation mechanism of the zeolite molecular sieves was explored through the changes of the silica-alumina during zeolite formation. This paper is the first to use the hydrothermal conversion of zeolite molecular sieves from LFS-FA based polymers to provide some guidance for the resource utilization of LFS and FA.
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