Immobilization mechanism of cesium in geopolymer: Effects of alkaline activators and calcination temperature.

Geopolymer is always regarded as a promising material for the immobilization of radioactive waste. In the present study, the stabilization of Cs in geopolymers activated by NaOH and NaSiO solutions and calcined at various temperatures was studied via toxicity characteristic leaching procedure (TCLP), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscope and energy dispersive spectroscopy (SEM-EDS), solid-state nuclear magnetic resonance (SSNMR), and N adsorption-desorption isotherm. For both NaOH-activated and NaSiO-activated geopolymers, the leaching concentrations of Cs decreased with the increase of calcination temperature. Specifically, most of the amorphous substance was crystallized to nepheline at 1000 °C for NaOH-activated geopolymer, and Cs can be incorporated into the structure of nepheline, contributing to the reduction of Cs leaching concentration. However, the amorphous structure was still maintained for NaSiO-activated geopolymer even after calcination at 1000 °C. It has been deduced that the main structure of NaSiO-activated geopolymer after calcination at 1000 °C should be in short-range order and Cs can be locked in a micro "crystal" structure. In addition, the change of specific surface area was not fully consistent with the decreasing trend of Cs leaching concentration. Therefore, the inner structure and the specific surface area of geopolymer should have a combined effect on the leaching behavior of Cs. This study can provide new insights into the application of geopolymer to immobilize radionuclides.