Abstract
Selective removal of 99TcO4− from complex radioactive wastewater is a challenging but meaningful task since it is important for both spent fuel reprocessing and 99TcO4− leakage handling. Here, we synthesized a series of functionalized PAF-1 framework materials, PAF-1-C-N2, PAF-1-N2-C4, PAF-1-IM and PAF-1-PY, by grafting quaternary ammonium, imidazolium and pyridinium onto the PAF framework as active sites, respectively, which purpose is to screen functional groups with high affinity for TcO4−. The structures and morphological characteristics of the four adsorbents were characterized by N2 adsorption-desorption, Fourier transform infrared spectroscopy (FT-IR), and scanning electron microscope (SEM). These materials exhibit high selectivity for TcO4−/ReO4−, rapid adsorption kinetics (reaching equilibrium within 30 s), and a wide pH range (pH 3–11) for ReO4−/TcO4−adsorption. Among them, PAF-1-IM had the best adsorption performance, and the partition coefficient K d reached 1.27 × 106 mL/g. 97.1 % and 96.9 % of ReO4− could be removed by PAF-1-IM even when the concentrations of PO43− and SO42− are 1000 times the concentration of ReO4−, respectively. When the solid-liquid ratio is 10 g/L, 93.7 % of TcO4− can be removed from the simulated Low Active Wastewater (LAW), which is higher than most other TcO4− adsorbents. X-ray energy dispersive spectroscopy (EDS) and FT-IR suggest the adsorption process was anion exchange.
Funding source: National Natural Science Foundation of China
Award Identifier / Grant number: 21976075
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Research ethics: Not applicable.
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Author contributions: The authors have accepted responsibility for the entire content of this manuscript and approved its submission.
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Competing interests: The authors state no conflict of interest.
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Research funding: This work was supported by the National Natural Science Foundation of China (21976075).
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Data availability: The raw data can be obtained on request from the corresponding author.
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Supplementary Material
This article contains supplementary material (https://doi.org/10.1515/ract-2023-0218).
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