Predicting the aggregation tendency of nanoscale zero-valent iron (nZVI), oxidized nZVI, in particular, is crucial for the risk assessment of nZVI in aquatic environments. In this study, the comprehensive effects of the pH and ionic strength (IS) on the aggregation behaviors of two highly oxidized nZVIs (HO-nZVI) were examined. Compared with hematite nanoparticles, HO-nZVI presented a sudden acceleration in aggregation under critical conditions; moreover, the morphology of the HO-nZVI aggregates at pH and IS values higher or lower than the critical conditions was significantly different. Furthermore, owing to the differences in magnetization between the two prepared HO-nZVI samples, their critical coagulation conditions were significantly different. The significant changes in the aggregation behavior of the HO-nZVI samples were analyzed using colloidal theories, and the aggregation tendency of HO-nZVI under specific conditions could be simulated by calculating the theoretical critical conditions of aggregation via a method that takes into account the hydrochemical properties, magnetization, and surface charge of HO-nZVI. To examine the correctness of the method, we compared the experimentally determined colloidal stability of HO-nZVI in water samples collected from nearby rivers with the theoretically predicted value. The results indicated that the method was adequate for most situations, except for those in which the hydrochemical properties of the water samples were close to the critical coagulation conditions. Our study proposes a theoretical approach that is viable for simulating the colloidal stability of magnetic nanoparticles in aquatic environments; we anticipate that it will further facilitate the risk assessment of nanoparticles.
Keywords: Aggregation behavior; Extended Derjaguin–Landau–Verwey–Overbeek theory; Oxidized nanoscale zero-valent iron; Simulation.