Fullerene nanoparticles exhibit greater retention in freshwater sediment than in model porous media

摘要

Increasing production and use of fullerene-based nanomaterials underscore the need to determine their mobility in environmental transport pathways and potential ecological exposures. This study investigated the transport of two fullerenes (i.e., aqu/C_(60) and water-soluble C_(60) pyrrolidine tris-acid [C_(60) PTA]) in columns packed with model porous media (Iota quartz and Ottawa sand) and a sediment from Call's creek under saturated and unsaturated steady-state flows. The fullerenes had the least retention in Iota quartz, and the greatest retention in the sediment at near neutral pH, correlating with the degree of grain surface chemical heterogeneity (e.g., amorphous Al hydroxides concentration increasing in the order of Iota quartz < Ottawa sand < sediment). Surface roughness was elucidated as another important factor responsible for the greatest fullerene retention in the sediment. In accordance with the XDLVO energy calculations, C_(60) PTA was less retained than aqu/C_(60) at near neutral pH, due to its greater hydrophilicity measured by tolune-water partition coefficient, as well as smaller particle sizes revealed by atomic force microscopy. Fullerene retention exhibited a strong dependency on solution pH that could be explained partly by the pH-dependent surface charge of fullerenes and grain surface, and partly by increased hydrophobicity of C_(60) PTA when solution pH approaches its isoelectric point (IEP). Finally, fullerene retention was enhanced in unsaturated media, implying that fullerenes may be more attenuated in the vadose zone than in groundwater.