Influence of natural organic matter on fate and transport of silver nanoparticles in saturated porous media: laboratory experiments and modeling

摘要

Understanding the fate and transport of silver nanoparticles (AgNPs) is of importance due to their widespread use and potential harmful effects on humans and the environment. The present study investigates the fate and transport of widely used Creighton AgNPs in saturated porous media. Previous investigations of AgNP transport in the presence of natural organic matter (NOM) report contradictory results regarding how the presence of NOM affected the stability and mobility of AgNPs. In this work, a nonreactive tracer, AgNPs and a mixture of AgNPs and NOM were injected into a background solution (0.01 mM of NaNO3) flowing through laboratory columns packed with water-saturated glass beads to obtain concentration versus time breakthrough curves. Transport of AgNPs in the presence of NOM was simulated with a model that accounted for both reversible and irreversible attachment. Based upon an analysis of the AgNP breakthrough curves, it was found that addition of NOM at concentrations ranging from 1 to 40 mg L-1 resulted in significant decreases in both the zeroth and first moments of the breakthrough curves. These observations may be attributed to NOM promoting AgNP aggregation and irreversible attachment. Raman and surface-enhanced Raman scattering analysis of NOM-AgNP mixtures revealed that a possible interaction of NOM with AgNP occurred through the carboxylic moieties (-COO-) located in the immediate vicinity of the metallic surface. At higher concentrations of NOM, both the zeroth and first moments of the breakthrough curves increased. Based on modeling and the literature, we hypothesize that as the NOM concentration increases, it begins to coat both the AgNPs and the glass beads, leading to a situation where AgNP transport may be described in the same way that transport of a sorbing hydrophobic compound partitioning to an immobile organic phase is typically described, assuming reversible, rate-limited sorption.