Immobilization of cesium in fly ash-silica fume based geopolymers with different Si/Al molar ratios.

Geopolymers are considered as promising matrixes for waste solidification. However, the effects of the Si/Al molar ratio of geopolymer on the immobilization efficiencies for metal ions have not been fully studied and understood. In the present study, geopolymers with different Si/Al ratios were synthesized from coal fly ash and silica fume. Adsorption tests were conducted to evaluate their immobilization efficiencies for Cs+. The results indicated that geopolymer with low Si/Al ratio could have a better immobilization performance for Cs+ than that with high Si/Al ratio. High Si/Al ratio could contribute to a more compact structure of geopolymer. Each sorption process fitted better with the pseudo-second-order model, and all of them were governed by film diffusion. However, the diffusion mode was gradually closed to particle diffusion with the increase in the Si/Al ratio. Both Langmuir and Freundlich models could well fit the sorption data, and the free energy of each sorption process decreased with the increase in the Si/Al ratio according to D-R equation. The distribution of AlO4 tetrahedron in the geopolymer structure plays a significant role in the immobilization of Cs+. Low Si/Al ratio could result in that more AlO4 tetrahedrons distribute in the small rings (

Reduction of undesirable element leaching from fly ash by adding hydroxylated calcined dolomite.

Fly ash always contains many toxic elements which can be released into environment, thereby easily leading to environmental contaminations. In order to dispose fly ash safely, related strategies are needed. In this investigation, two kinds of hydroxylated calcined dolomites (HCD60 and HCD100) were used as the additives and compared with lime on the leachabilities of anionic species from fly ash. Both additives were found effective in reducing the leaching concentrations of these elements, which was better than that of only lime addition. Mg(OH)2 and MgO were believed to play important roles in the hydration reaction of fly ash. In the presence of Mg(OH)2 and MgO, there were more hydration products including calcium silicate hydrate, ettringite, hydrocalumite and other Layered double hydroxides (LDHs) generated which were effective candidates for anion removal. Thus, the final leaching results were controlled by these newly formed phases through adsorption, incorporation or encapsulation. On the other hand, compared with Mg(OH)2, MgO can promote the formation of hydration products in a larger extent because of the hydration process of MgO into Mg(OH)2. There was no systematic trend in the promotion of fly ash hydration by Mg(OH)2 or MgO because it had a close relationship with the properties of original fly ash. Objectively, hydroxylated calcined dolomites can be promising candidate additives for reduction of toxic elements leaching from fly ash.

Suppression processes of anionic pollutants released from fly ash by various Ca additives.

Harmful trace elements, which are initially included in the coal fly ash, have the potential to be leached when coal fly ash comes in contact with water. This causes a risk of pollutant species being released, considering the long lifetime of building structures where coal fly ash was applied. Some Ca additives effectively function to suppress the release of anionic pollutants; however, the detailed suppression processes remains unclear. In this work, the influences of various Ca additives on the released anionic pollutants (B, F, S, As, and Cr) was systematically investigated. According to the comprehensive results of solution data with the solid characterization, the 60% hydroxylated calcined dolomite (HCD 60) was the best Ca additive for the suppression of different anionic pollutants since this Ca source not only simply provides an alkaline reagent but also supplies MgO and Mg(OH)2, which affect the phase transformation that accompanies with hydration. The phase transformation occurs from Ca(OH)2 to ettringite via hydrocalumite, which is the most important suppression processes of released pollutants. The precipitation of Ca salts is another pathway to immobilize these pollutants. In this scheme, MgO and Mg(OH)2 were proven to enhance the formation of ettringite and hydrocalumite, respectively.

Distributions and Leaching Behaviors of Toxic Elements in Fly Ash.

Fly ash usually contains a considerable amount of toxic elements that can be leached into the environment, thereby easily leading to serious contaminations. In this work, the leaching behaviors of poisonous elements including boron (B), phosphorus (P), vanadium (V), chromium (Cr), arsenic (As), selenium (Se), molybdenum (Mo), antimony (Sb), and tungsten (W) from fly ash were explored by sequential extraction. Importantly, the associations of these elements in fly ash were discussed based on their leaching and X-ray absorption near-edge structure (XANES) results. From the XANES results, it was observed that V(IV), Cr(III), As(V), Se(IV), and W(IV) were their main states of existence in fly ash. In terms of leaching results, large amounts of Mo and W were leached into pure water, which indicated their high mobilities. Furthermore, the occurrence of Mo in fly ash was mainly in the form of oxides, and W had complex associations including WX4 (X can be monovalent anions), its reduction state or association with the elements that can be oxidized, and existence in silicates. B was as easily released into the environment as Mo and W. It can have several associations with the other cations, such as Ca2+, Na+, and Mg2+, and occurs in silicates. In contrast, most of the Cr and Sb were locked in silicates, indicating that they were very stable in fly ash. In addition, P, V, and As can exist within the structure of silicates as well. However, a considerable amount of them leached in the reduction step with a low pH. Hence, they can be associated with Ca2+, Na+, Mg2+, or Fe3+. In terms of Se, oxidation processes played an important role in controlling its leaching because of the oxidation of Se(IV) to Se(VI). Calcium selenite should be the predominant form of Se in fly ash.