Effective removal of heavy metal complexes from contaminated water remains a challenging task. In this work, a limestone/PMS system was constructed for the efficient degradation of Cu-EDTA. Under the conditions of 3.0 g/L limestone and 1.0 mM PMS, the degradation efficiency of 10.0 mg/L Cu-EDTA reached 99.0 % in 60 min, and the removal efficiency of Cu ions approached 50.0 %. The main active specie revealed by quenching and EPR experiments was the singlet oxygen (1O2). Interestingly, Trace amounts of Cu(II) in limestone react with PMS enhancing the degradation of Cu-EDTA. The results of the HPLC-MS analysis showed that the reactive species attacked the Cu–O and Cu–N bonds, as well as triggered a decarboxylation process, resulting in the decomposition of Cu-EDTA into six intermediates. Meanwhile, SEM and XPS analyses revealed that Cu ions released during the degradation of Cu-EDTA are deposited on the limestone surface as Cu(OH)2 and Cu2(OH)2CO3. In addition, the initial pH and co-existing ions have a weak effect on the system. Finally, a one-month continuous flow experiment showed that the degradation efficiency of Cu-EDTA was about 95.0 % and the removal efficiency of Cu ions was 40.0 %. In conclusion, this study provides a new approach for the destruction of metal complexes and the removal of heavy metals.
Read full abstract