Enhanced Heterogeneous Fenton-like Degradation of Nuclear-grade Cationic Exchange Resin by Nanoscale Zero-valent Iron: Experiments and DFT Calculations
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Toxicology
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Nanoscale zero-valent iron (nZVI) was prepared and used as a heterogeneous Fenton-like catalyst for the degradation of nuclear-grade cationic exchange resin. The properties of nZVI before and after reaction were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), and Brunauer-Emmett-Teller (BET) surface area analysis. The results showed that nZVI-HO system exhibited the enhanced degradation of cationic resins, compared with Fe-HO, Cu-HO, and Fe/Cu-HO systems. The effects of initial temperature, nZVI dose, and HO concentration were studied, and the higher temperature and nZVI dose with relatively low HO concentration brought faster degradation rate. The degradation of cationic resins followed the pseudo-first-order kinetics with the apparent activation energy of 53.29 kJ/mol. According to the experimental and calculated infrared and UV-visible spectra, the carbon skeleton of cationic resins was broken with the detachment of benzene ring and the desulfonation of resin polymer by hydroxyl radicals (•OH), generating long-chain alkenes. These intermediates were further oxidized through the hydroxyl substitution, hydrogen abstraction, ring cleavage, or carbonylation reactions, finally forming carboxylic acids remained in solution.