Technetium-99 decontamination from radioactive wastewater by modified bentonite: batch, column experiment and mechanism investigation

CHEMICAL ENGINEERING JOURNAL(2022)

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摘要
Technetium-99 (99Tc), as one of the important high-yield fission products, poses a significant threat to the environment and human health due to its radiotoxicity, long half-life, high solubility and mobility in the environment. Thus, removal of 99TcO4xfffd; from radioactive wastewater is considerably imminent for waste disposal and environment conservation. In this work, Hexadecylpyridinium Chloride Monohydrate modified bentonite (HDPy-bent) was synthesised and used as an adsorbent to remove 99TcO4xfffd; . The adsorption behaviours of ReO4xfffd; as an analogue for TcO4xfffd; were investigated as functions of contact time, solution pH, initial concentration, and competing anions using batch techniques. It is demonstrated that the HDPy-bent showed an excellent adsorption ability for ReO4xfffd; at the pH range of 2-11, fast adsorption kinetic (reaching equilibrium within 3 min at room temperature), and maintains desirable ReO4xfffd; adsorption in the presence of concomitant anions at an excessive concentration of 500 times (Clxfffd;, HCO3xfffd;, NO3xfffd;, CO32 , SO42xfffd; and PO43xe213; ). As for adsorption mechanism, we propose the anion exchange process at low concentration of Re(VII) and precipitation reaction at high concentration, while the driving force of the high ReO4xfffd; adsorption ability is the interaction between ReO4xfffd; anion and pyridinium ring of HDPy+, which is confirmed by density functional theory (DFT) simulations. Additionally, DFT studies also shed light on the adsorption structure of HDPy+/ReO4xfffd; and the origin of adsorption selectivity. Moreover, four adsorption-desorption cycles suggest that the HDPy-bent has good durability and reusability. Furthermore, ReO4xfffd; can be removed completely and recovered fractionally by using the chromatography column packed with HDPy-bent from simulated groundwater samples. The work presented herein demonstrates a lowcost adsorbent which can efficiently remove 99Tc from contaminated water.
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关键词
Tc-99, HDPy-bent, Adsorption mechanism, Density functional theory, Column experiment
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