Mechanism and controlling factors on rapid methylmercury degradation by ligand-enhanced Fenton-like reaction at circumneutral pH

Methylmercury (MeHg), derived from industrial processes and microbial methylation, is still a worldwide environmental concern. A rapid and efficient strategy is necessary for MeHg degradation in waste and environmental waters. Here, we provide a new method with ligand-enhanced Fenton-like reaction to rapidly degrade MeHg under neutral pH. Three common chelating ligands were selected (nitriloacetic acid (NTA), citrate, and ethylenediaminetetraacetic disodium (EDTA)) to promote the Fenton-like reaction and degradation of MeHg. Results showed that MeHg can be rapidly degraded, with the following efficiency sequence: EDTA > NTA > citrate. Scavenger addition demonstrated that hydroxyl radical (▪OH), superoxide radical (O2▪–), and ferryl (FeⅣO2+) were involved in MeHg degradation, and their relative contributions highly depended on ligand type. Degradation product and total Hg analysis suggested that Hg(Ⅱ) and Hg0 were generated with the demethylation of MeHg. Further, environmental factors, including initial pH, organic complexation (natural organic matter and cysteine), and inorganic ions (chloride and bicarbonate) on MeHg degradation, were investigated in NTA-enhanced system. Finally, rapid MeHg degradation was validated for MeHg-spiked waste and environmental waters. This study provided a simple and efficient strategy for MeHg remediation in contaminated waters, which is also helpful for understanding its degradation in the natural environment.