Top-Down Synthesis of NaP Zeolite from Natural Zeolite for the Higher Removal Efficiency of Cs, Sr, and Ni

Abstract

A solid phase of natural zeolite was transformed to Na-zeolite P (NaP zeolite) by a “top-down approach” hydrothermal reaction using 3 M of NaOH solution in a 96 °C oven. Time-dependent X-ray diffraction (XRD), Fourier-transform infrared (FT-IR), XRF, and scanning electron microscopy (SEM) analysis as well as kinetic, isotherm, and cation exchange capacity experiments were performed to understand the mechanism of mineral transition from natural zeolite to NaP zeolite. The XRD crystal peaks of the natural zeolite decreased (decrystallization phase) first, and then the NaP zeolite XRD crystal peaks increased gradually (recrystallization phase). From the XRF results, the dissolution rate of Si was slow in the recrystallization phase, while it was rapid in the decrystallization phase. The specific surface area measured by BET analysis was higher in NaP zeolite (95.95 m2/g) compared to that of natural zeolite (31.35 m2/g). Furthermore, pore structure analysis confirmed that NaP zeolites have more micropores than natural zeolite. In the kinetic experiment, the results showed that the natural zeolite and NaP zeolite were well matched with a pseudo-second-order kinetic model, and reached equilibrium within 24 h. The isotherm experiment results confirmed that both zeolites were well matched with the Langmuir isotherm, and the maximum removal capacity (Qmax) values of Sr and Ni were highly increased in NaP zeolite. In addition, the cation exchange capacity (CEC) experiment showed that NaP zeolite has an enhanced CEC of 310.89 cmol/kg compared to natural zeolite (CEC = 119.19 cmol/kg). In the actual batch sorption test, NaP zeolite (35.3 mg/g) still showed high Cs removal efficiency though it was slightly lower than the natural zeolite (39.0 mg/g). However, in case of Sr and Ni, NaP zeolite (27.9 and 27.8 mg/g, respectively) showed a much higher removal efficiency than natural zeolite (4.9 and 5.5 mg/g for Sr and Ni, respectively). This suggests that NaP zeolite, synthesized by a top-down desilication method, is more practical to remove mixed radionuclides from a waste solution.