Zirconosilicate Sorbent Based on Coal Fly Ash Cenospheres for Cesium Immobilization in a Ceramic Form

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Resumo

Hollow aluminosilicate microspheres (cenospheres) of stabilized composition (glass phase – 95.4 wt. %; (SiO2/Al2O3)glass – 3.1) isolated from fly ashes from coal combustion were used to prepare composite sorbents containing a sorption-active component based on zirconosilicates of framework structure. The synthesis products were characterized by XRD, SEM-EDS and low-temperature nitrogen adsorption methods, and their sorption properties towards Cs+ were studied. Zirconosilicate material demonstrates the high distribution coefficient in the process of Cs+ sorption from aqueous solutions (~103–104 ml/g) and stability of sorption capacity as a result of decationation. The possibility of application of SPS-synthesis technology to create high-density mineral-like ceramics for cesium immobilization based on the zirconosilicate sorbent has been investigated. The results of dilatometry, structure and porosity analyses were obtained for ceramics sintered at different temperatures (800–1000°C).

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Sobre autores

T. Vereshchagina

Krasnoyarsk Science Center of the Siberian Branch of the Russian Academy of Sciences; Siberian Federal University

Email: shichalin_oo@dvfu.ru
Rússia, Krasnoyarsk, 660036; Krasnoyarsk, 660041

E. Kutikhina

Krasnoyarsk Science Center of the Siberian Branch of the Russian Academy of Sciences

Email: shichalin_oo@dvfu.ru
Rússia, Krasnoyarsk, 660036

O. Buyko

Siberian Federal University

Email: shichalin_oo@dvfu.ru
Rússia, Krasnoyarsk, 660041

A. Belov

Far Eastern Federal University

Email: shichalin_oo@dvfu.ru
Rússia, Russky Island, Vladivostok, 690922

O. Shichalin

Far Eastern Federal University; Sakhalin State University

Autor responsável pela correspondência
Email: shichalin_oo@dvfu.ru
Rússia, Russky Island, Vladivostok, 690922; Yuzhno-Sakhalinsk, 693000

A. Anshits

Krasnoyarsk Science Center of the Siberian Branch of the Russian Academy of Sciences

Email: shichalin_oo@dvfu.ru
Rússia, Krasnoyarsk, 660036

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2. Fig. 1. Heteropolyhedral framework structure of the Na4Zr2(SiO4)3 phase of the NASICON family.

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3. Fig. 2. SEM images of the narrow fraction of cenospheres.

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4. Fig. 3. SEM images of zeolitisation (a) and zeolitisation-de-alumination (b) products of initial cenospheres; surface areas of modified cenospheres according to EDS data (c, d).

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5. Fig. 4. SEM images (a, b) and diffractogram (d) of hydrothermal synthesis products in the system ZrOCl2-NaOH-H2O-(H, Na)X; surface area of product pellets according to EDS data (c).

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6. Fig. 5. Low-temperature nitrogen adsorption-desorption isotherm for the Zr-Si/NASICON sample (a) and pore width distribution calculated from the adsorption branch (b), in dV/dw-lgw coordinates.

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7. Fig. 6. Cs+ sorption isotherms for synthesis products based on NASICONA phases (dots - experiment, lines - Langmuir model).

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8. Fig. 7. Samples of zirconosilicate-based ceramic materials obtained by IPS-synthesis at temperatures from 800 to 1000°C.

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9. Fig. 8. Dilatometric dependences of ceramics obtained at different temperatures by the EIPS method.

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10. Fig. 9. SEM images of ceramic samples obtained by EIPS at 800°C (a, b), 900°C (c, d) and 1000°C (e, f); distribution maps of Zr, Si and Cs in ceramics obtained at 800°C (g).

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11. Fig. 10. Diffractograms of ceramics obtained at different temperatures.

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12. Fig. 11. Low-temperature nitrogen adsorption-desorption isotherms for samples obtained at different sintering temperatures (a) and pore width distribution calculated from the adsorption branch (b), in dV/dw-lgw coordinates.

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