Due to the highly acidic and high-salinity nature of the high-level radioactive waste liquid (HLLW), selective extraction of TcO from HLLW remains to be a challenging task. Traditional anion exchangers show low selectivity and unsatisfactory extraction performance due to the lack of functional groups that can interact strongly with TcO. In this work, a tailor-made binding site was constructed by decorating two acetamide functional groups on imidazolium cation to fabricate a new Tc separation material, which exhibits high selectivity. Unlike most reported Tc separation materials, which can only perform well under low acidic, neutral, or alkaline conditions, this material still has good extraction performance in highly acidic solutions. In the simulated high-level waste liquid of 3 M nitric acid, the extraction efficiency of 0.5 mol/L organic phase for Tc can reach 96.5% through the first-stage extraction. Our theoretical simulations suggest that ReO/TcO anions were adsorbed on the top of the imidazolium ring during the extraction process, with p-π and p-p interactions acting as the driving forces.
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http://dx.doi.org/10.1021/acs.inorgchem.2c01775 | DOI Listing |
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