The Application of Iron(III)-Tetraamidomacrocyclic Ligand/Peroxide System for Rapid In-situ Degradation of Groundwater Bisphenols
摘要
In this study, an iron(III)-tetraamidomacrocyclic ligand (Fe(III)-TAML)/peroxide system was developed to degrade bisphenols in groundwater. The results demonstrated that this system effectively degrades both bisphenol A (BPA) and bisphenol AF (BPAF), with optimal degradation occurring at pH 10 and 9, respectively. The system’s efficiency can be attributed to the increased proportion of deprotonated Fe(III)-TAML species at higher pH levels. These species are more reactive and can be easily oxidized by hydrogen peroxide (H₂O₂) or peroxymonosulfate (PMS) to form highly reactive Fe(IV)-TAML or Fe(V)-TAML, which drive the degradation process. Notably, the Fe(III)-TAML/PMS system outperformed the Fe(III)-TAML/H₂O₂ system, especially under near-neutral pH conditions. The degradation pathways involved initial electron-deficient reactions at the hydroxyl groups of bisphenols, leading to the formation of phenoxy radicals. Subsequent steps included resonance stabilization, β-scission, and further oxidation. The final degradation products were identified as low-molecular-weight organic acids with significantly reduced acute and chronic toxicities. This highlights the environmental friendliness of the Fe(III)-TAML/peroxide system. Overall, this study provides a promising approach for the rapid and efficient degradation of bisphenols in groundwater, offering a potential solution to mitigate the environmental risks associated with these contaminants.