Fast removal of uranium from aqueous solutions using tetraethylenepentamine modified magnetic chitosan resin
Introduction
The mining of uranium ores and their hydrometallurgical processing as well as the operation of nuclear power plants and disposal of spent nuclear fuel are potential sources of radioactive pollution of the environment. About 40,000–50,000 tons of uranium are produced every year (OECD Nuclear Energy Agency, 2010). Uranium is considered to be not only an irreplaceable raw material for nuclear energy, but also a serious long-term potential environmental hazard (Zhang et al., 2011). Uranium ions often accumulate in both water and the environment because of its long half-life. Hence, its presence poses an environmental challenge. Over the past few decades, a variety of technologies including chemical and biological precipitation (Kim et al., 2011, Zhang et al., 2013), solvent extraction (Quinn et al., 2013), ion exchange (Pulhani et al., 2012), membrane processes (Kedari et al., 2013), and adsorption (Cao et al., 2013, Katsoyiannis and Zouboulis, 2013) have been developed for the removal and recovery of uranium from nuclear fuel effluents, mine tailings, seawater and other waste sources. Lately, adsorption, due to its high-efficiency and readily handling has been gradually utilized (Katsoyiannis and Zouboulis, 2013). Therefore, the design and preparation of adsorbents with low cost and high-stability, efficiency and selectivity has been drawing considerable interests in processing uranium recovery and decontamination.
Chitin is one of the most abundant polysaccharides after cellulose. It is a basic structural component of fungal and yeast cell walls, as well as of numerous invertebrates (Muzzarelli et al., 2012). Chitosan, the linear (1,4)-2-amino-2-deoxy-β-d-glucan, can be obtained from chitin by partial deacetylation. These biopolymers are potent sorbents for various transition metals and radionuclides (Guibal et al., 2009, Schleuter et al., 2013). Grafting of new functional groups and chemical crosslinking of chitosan increases its adsorption capacity, stability and/or selectivity towards metal ions through the formation of different chelates.
The ultimate goal of this study is the development of magnetic chitosan resin bearing supplementary amine groups for the removal of ions from aqueous solution. These methods are cheap and often highly scalable. Moreover, techniques employing magnetism are more amenable to automation (Atia et al., 2008). Magnetic separation techniques offer several advantages. The most attractive one for radioactive wastewater treatment is its good performance in difficult-to-handle samples. By using the magnetic separation techniques rather than centrifugation or filtration, it will reduce the chances of contacting with radiations. However, so far only limited knowledge exists concerning the removal of radioactive substances by magnetic separation method, especially uranium removal by magnetically modified chitosan, which is meaningful from the purification, environmental and radioactive waste disposal point of view.
To address this objective in this study we use chitosan modified with magnetite and tetraethylenepentamine (TEPA) for removal from aqueous media. U(VI) adsorption onto the TEPA-magnetic chitosan was investigated, including (a) pH optimization, (b) determination of sorption isotherms and uptake kinetics in batch system, and (c) evaluation of breakthrough curves (in fixed bed column).
Section snippets
Chemicals
Chitosan (M.W. 190,000–310,000 Da), glutaraldehyde, tetraethylenepentamine (TEPA) were Sigma–Aldrich products. Arsenazo-III (M.W. 892.4) was procured from Himedia (Mumbai, India). All other chemicals were Prolabo products and were used as received. Uranyl chloride was used as the source of ions. FeSO4·7H2O and FeCl3·6H2O were used for preparing magnetite particles as reported earlier using modified Massart method (Qu et al., 1999). 2.07 g of FeCl3·6H2O and 0.81 g of FeCl2·4H2O were dissolved
Morphology study
The morphology of TEPA@MCHS beads was examined using scanning electron microscopy (SEM). The SEM micrographs of the raw TEPA@MCHS show a coarse surface with several small pores inside and suggest interconnected macropores within the resin (Fig. AM1 a,b,c, See Additional Material Section). However, apparent differences in the surface morphologies of the adsorbent after adsorption were observed (Fig. AM1 d,e,f, See Additional Material Section). The surface was changed to smooth with many
Conclusion
Resin TEPA@MCHS is characterized by fast and highly efficient adsorption towards ions at optimum pH (i.e., pH 4). The uptake kinetic was described by the PSORE. The sorption isotherm is modeled by the Langmuir equation. The maximum sorption capacity reached 1.67 mmol g−1at 25 °C. Column studies give an account about the breakthrough points at different flow rates and bed heights. The critical bed height of the resin towards was found to be 0.926 cm at flow rate of 4 mL/min. The
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