Enhanced heterogeneous Fenton-like degradation of nuclear-grade cationic exchange resin by nanoscale zero-valent iron: experiments and DFT calculations
2020
Xu, Lejin | Sun, Peijie | Meng, Xiang | Shen, Huiyi | Li, Wuyang | Wang, Jianlong | Yang, Jun
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–H₂O₂ system exhibited the enhanced degradation of cationic resins, compared with Fe²⁺–H₂O₂, Cu⁰–H₂O₂, and Fe⁰/Cu⁰–H₂O₂ systems. The effects of initial temperature, nZVI dose, and H₂O₂ concentration were studied, and the higher temperature and nZVI dose with relatively low H₂O₂ 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.
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