Total mercury and methylmercury migration and transformation in an A/O wastewater treatment plant.

Municipal wastewater treatment plants (MWTPs) serve an essential role in reducing mercury (Hg) pollution. However, few studies quantified the transport and transformation of Hg through MWTPs, particularly plants based on the anaerobic-anoxic-aerobic (A/O) process. Here, we present a mass balance for total mercury (THg) and total methylmercury (TMeHg) at the plant, and investigate the influence of pH, temperature, and dissolved oxygen on the occurrence and fate of methylmercury (MeHg) in the system. The concentrations of the THg and TMeHg in the raw sewage were 40.3 ± 26.6 ng/L (4.3 ± 2.7 g/day) and 1.9 ± 0.6 ng/L (193 ± 58 mg/day), respectively. Their concentrations in the plant's effluent water were 7.4 ± 1.5 ng/L (0.74 ± 0.2 g/day) and 0.04 ± 0.01 ng/L (3.9 ± 1.0 mg/day), corresponding to decreases of ~82% for THg and ~98% for TMeHg. Within the plant, only ~10% of the THg was removed with primary sedimentation, as Hg in the raw sewage was predominately in dissolved form. In contrast, a significant portion of TMeHg (~43%) was associated with incoming particulate matter. Much of the remaining Hg was removed in subsequent A/O process and secondary clarifiers, with a ~78% of the THg entering the plant transferring to the dewatered sludge (concentration 1.05 ± 0.28 μg/g; 3.2 ± 0.8 g/day). These same steps decreased TMeHg in the water by ~95%, with <10% of that reduction being TMeHg transferred to the sludge (concentration 2.1 ± 1.1 ng/g; 6.2 ± 3.3 mg/day), suggesting >90% TMeHg degradation. In addition, the most important factor that impacted the variation of TMeHg concentrations was pH, then was temperature. Dissolved oxygen showed no relationship with TMeHg and DMeHg. Overall, this study demonstrates that A/O MWTPs effectively remove MeHg from wastewater, however, sludge remains an important potential source of Hg to the environment.