RESUMEN
Capture and immobilization of 137Cs is urgent for radioactive contamination remediation and spent fuel treatment. Herein, an effective all-in-one treatment method to simultaneously adsorb and immobilize Cs+ without high-temperature treatment is proposed. According to the strategy of incorporating high-valency metal ions into molybdates to increase the material stability and affinity towards radionuclides, layered HMMoO6·nH2O (M = Ta (1), Nb (2)) are prepared. Both materials exhibit excellent acid resistance (even 15 mol/L HNO3). They maintain remarkable adsorption capacity for Cs+ in 1 mol/L HNO3 solutions and can selectively capture Cs+ under excessive competitive ions. Furthermore, they show successful cleanup for actual 137Cs-liquid-wastes generated during industrial production. In particular, adsorbed Cs+ can be firmly immobilized in interlayer spaces of materials due to the highly stable anionic framework. The removal mechanism is attributed to ion exchange between Cs+ and interlayer H+ by multiple characterizations. Study of the structure-function relationship shows that the occurrence of Cs+ ion exchange is closely related to plate-like layered structure. This work develops an efficient all-in-one treatment method for capturing and immobilizing radiocesium by ultra-stable inorganic solid acid materials with low energy consumption and high safety for radionuclide remediation.
RESUMEN
137 Cs and 90 Sr are hazardous to ecological environment and human health due to their strong radioactivity, long half-life, and high mobility. However, effective adsorption and separation of Cs+ and Sr2+ from acidic radioactive wastewater is challenging due to stability issues of material and the strong competition of protons. Herein, a K+ -activated niobium germanate (K-NGH-1) presents efficient Cs+ /Sr2+ coadsorption and highly selective Cs+ /Sr2+ separation, respectively, under different acidity conditions. In neutral solution, K-NGH-1 exhibits ultrafast adsorption kinetics and high adsorption capacity for both Cs+ and Sr2+ (qm Cs = 182.91 mg g-1 ; qm Sr = 41.62 mg g-1 ). In 1 M HNO3 solution, K-NGH-1 still possesses qm Cs of 91.40 mg g-1 for Cs+ but almost no adsorption for Sr2+ . Moreover, K-NGH-1 can effectively separate Cs+ from 1 M HNO3 solutions with excess competing Sr2+ and Mn + (Mn + = Na+ , Ca2+ , Mg2+ ) ions. Thus, efficient separation of Cs+ and Sr2+ is realized under acidic conditions. Besides, K-NGH-1 shows excellent acid and radiation resistance and recyclability. All the merits above endow K-NGH-1 with the first example of niobium germanates for radionuclides remediation. This work highlights the facile pH control approach towards bifunctional ion exchangers for efficient Cs+ /Sr2+ coadsorption and selective separation.