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 Na2SiO3 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 N2 adsorption-desorption isotherm. For both NaOH-activated and Na2SiO3-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 Na2SiO3-activated geopolymer even after calcination at 1000 °C. It has been deduced that the main structure of Na2SiO3-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.

Influence of aluminate and silicate on selenate immobilization using alkaline-earth metal oxides and ferrous salt.

Effects of aluminate and silicate species on the SeO42- immobilization using alkali-earth metal oxides and ferrous species have not been clearly elucidated. In the present study, Al and Si species were separately added into MgO/Fe(II) and CaO/Fe(II) reactions containing SeO42-, studied by toxicity characteristic leaching procedure (TCLP), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), X-ray absorption fine structure (XAFS), and PHREEQC simulation. Approximately 42 % of SeO42- was reduced to SeO32- for MgO/Fe(II) reaction in the presence of Al species, being consistent with the case without Al species. The Al species only showed slight inhibition of Se leaching for the MgO/Fe(II) reaction. Most of Se oxyanions were adsorbed onto Mg(OH)2 through outer-sphere complexation. For CaO/Fe(II) reaction, all of SeO42- was reduced to SeO32- with or without Al species. However, the Se leaching amount (3 %) of sample added with Al species (CE3) is much lower than that (12 %) of sample without Al species (CE2). This is mainly because SeO32- can be sorbed onto the iron-based minerals through binuclear bidentate corner-sharing (2C) complexation instead of monodentate mononuclear corner-sharing (1V) complexation of the case without Al species. On the other hand, SeO42- was not reduced to SeO32- in the presence of silicate, and almost all of Se was leached out for silicate-contained samples except CaO/Fe(II) reaction with the addition of Al species. This is due to the polymerization of Al and Si species under a high-alkalinity environment, thereby stabilizing SeO42- in the amorphous silicon-aluminum structure and contributing to the decrease of Se leaching.

A Bibliometric Analysis of Research Progress and Trends on Fly Ash-Based Geopolymer.

The objective of this work is to present the research progress and applications of fly ash-based geopolymer, and summarize the future research hotpots. Since 1998, scholars have made important contributions to the study of fly ash-based geopolymer, and a large number of research studies have been published. Therefore, a bibliometric analysis for the determination of the research status, trend, and history of fly ash-based geopolymer was conducted in the present study. A total of 4352 publications on fly ash-based geopolymer were collected between 1998 and 2022, with an increasing trend year by year. China and Australia are the largest contributors to the field, and the research institutions in each country cooperate closely. In addition, the most contributing research areas are MATERIALS SCIENCE, ENGINEERING, and CONSTRUCTION & BUILDING TECHNOLOGY. The keywords including fly ash, compressive strength, and mechanical property are the most frequently appearing words. On the whole, the development of fly ash-based geopolymer could be divided into three stages including the replacement of ordinary Portland cement, the development of multifunctional materials, and the reduction of environmental impact by the conversion of solid waste. This overview could provide an important guidance for the development of fly ash-based geopolymer.

Application of Geopolymer in Stabilization/Solidification of Hazardous Pollutants: A Review.

Geopolymers, as a kind of inorganic polymer, possess excellent properties and have been broadly studied for the stabilization/solidification (S/S) of hazardous pollutants. Even though many reviews about geopolymers have been published, the summary of geopolymer-based S/S for various contaminants has not been well conducted. Therefore, the S/S of hazardous pollutants using geopolymers are comprehensively summarized in this review. Geopolymer-based S/S of typical cations, including Pb, Zn, Cd, Cs, Cu, Sr, Ni, etc., were involved and elucidated. The S/S mechanisms for cationic heavy metals were concluded, mainly including physical encapsulation, sorption, precipitation, and bonding with a silicate structure. In addition, compared to cationic ions, geopolymers have a poor immobilization ability on anions due to the repulsive effect between them, presenting a high leaching percentage. However, some anions, such as Se or As oxyanions, have been proved to exist in geopolymers through electrostatic interaction, which provides a direction to enhance the geopolymer-based S/S for anions. Besides, few reports about geopolymer-based S/S of organic pollutants have been published. Furthermore, the adsorbents of geopolymer-based composites designed and studied for the removal of hazardous pollutants from aqueous conditions are also briefly discussed. On the whole, this review will offer insights into geopolymer-based S/S technology. Furthermore, the challenges to geopolymer-based S/S technology outlined in this work are expected to be of direct relevance to the focus of future research.

Immobilization of strontium in geopolymers activated by different concentrations of sodium silicate solutions.

Sodium silicate is always used as an activator for the synthesis of geopolymer. However, the effect of sodium silicate concentration on the geopolymer used as adsorbent was still unclear. Therefore, the immobilization of Sr2+ in geopolymers activated by different concentrations of sodium silicate was studied through kinetic and isotherm modeling and solid characterizations including XRD, FTIR, TG, SEM-EDS, and N2 adsorption-desorption isotherm. The adsorption amount of Sr2+ decreased with the sequence of S1, S2, and S3. According to the kinetic and isotherm modeling results, these sorption processes fitted better with pseudo-second-order, mainly governed by film diffusion. However, the diffusion mode was gradually closed to particle diffusion as for the sequence of S3, S2, and S1. Besides, the Langmuir model can be more befitting to sorption data than the Freundlich model, and the free energies decreased with the order of S1, S2, and S3. In addition, the specific surface areas did not change regularly with S1, S2, and S3. Thus, the distribution of Al tetrahedrons has a decisive role in the sorption process of Sr2+, even though the specific surface area is also a critical factor. More Al tetrahedrons can be formed under the activation of sodium silicate with higher concentration, leading to the low Si/Al molar ratio of the as-synthesized geopolymer.