Abstract
Where surface-functionalized engineered nanoparticles (NP) occur in drinking water catchments, understanding their transport within and between environmental compartments such as surface water and groundwater is crucial for risk assessment of drinking water resources. The transport of NP is mainly controlled by (i) their surface properties, (ii) water chemistry, and (iii) surface properties of the stationary phase. Therefore, functionalization of NP surfaces by organic coatings may change their fate in the environment. In laboratory columns, we compared the mobility of CeO2 NP coated by the synthetic polymer polyacrylic acid (PAA) with CeO2 NP coated by natural organic matter (NOM) and humic acid (HA), respectively. The effect of ionic strength on transport in sand columns was investigated using deionized (DI) water and natural surface water with 2.2 mM Ca2+ (soft) and 4.5 mM Ca2+ (hard), respectively. Furthermore, the relevance of these findings was validated in a near-natural bank filtration experiment using HA-CeO2 NP. PAA-CeO2 NP were mobile under all tested water conditions, showing a breakthrough of 60% irrespective of the Ca2+ concentration. In contrast, NOM-CeO2 NP showed a lower mobility with a breakthrough of 27% in DI and < 10% in soft surface water. In hard surface water, NOM-CeO2 NP were completely retained in the first 2 cm of the column. The transport of HA-CeO2 NP in laboratory columns in soft surface water was lower compared to NOM-CeO2 NP with a strong accumulation of CeO2 NP in the first few centimeters of the column. Natural coatings were generally less stabilizing and more susceptible to increasing Ca2+ concentrations than the synthetic coating. The outdoor column experiment confirmed the low mobility of HA-CeO2 NP under more complex environmental conditions. From our experiments, we conclude that the synthetic polymer is more efficient in facilitating NP transport than natural coatings and hence, CeO2 NP mobility may vary significantly depending on the surface coating.