4.7 Article

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

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 428, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.131333

Keywords

Tc-99; HDPy-bent; Adsorption mechanism; Density functional theory; Column experiment

Funding

  1. National Natural Science Foundation of China [21771093, 22061132004]
  2. Fundamental Research Funds for the Central Universities of China [lzujbky-2021-kb11]
  3. Gansu guiding program of Science and Technology Innovation [20JR10RA610]

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Technetium-99, a high-yield fission product, is a significant threat due to its radiotoxicity and high solubility in the environment. The study introduced a low-cost adsorbent, HDPy-bent, which showed excellent adsorption ability for ReO4, an analogue for TcO4, across a range of pH levels, demonstrating potential for efficient removal of 99Tc from contaminated water.
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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