Abstract
The thermally activated persulfate (TAP) advanced oxidation process is a promising technology for treating complex heavy–metal wastewater because of its environmental friendliness and high efficiency. However, previous studies have not fully explored the potential mechanisms involved in removing complex heavy metals. Herein, we investigated the effects of temperature, initial pH, peroxydisulfate (PDS) dosage, and the initial concentration of Ni-EDTA on the removal of Ni-EDTA using TAP. Results showed that increasing the activation temperature and PDS dosage enhanced the removal rate of Ni-EDTA, whereas decreasing the pH and initial concentration of Ni-EDTA were more conducive to Ni-EDTA removal. In addition, the quenching experiment indicated that OH and SO4− were the main active species, with OH being the most important contributor in the Ni-EDTA removal process. The degradation mechanism of Ni-EDTA was also explored through ultra performance liquid chromatography–mass spectrometry (UPLC–MS) analysis and density functional theory (DFT) calculations. These showed that the TAP-based degradation of Ni-EDTA is a step-by-step decarboxylation process due to increased bond lengths of CN or NCCN bonds of Ni-EDTA, resulting in the destabilization of Ni-EDTA. Overall, this study provides unique insights into the degradation of complex heavy metals in industrial wastewater using TAP.
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