Visualization and analysis of nanoparticle transport and ageing in reactive porous media

We present quasi-3D visualization and analysis of engineered nanoparticle (ENP) transport behavior in an experimental setup that uses a transmitted light imaging technique. A flow cell was packed with specially adapted, water-transparent, spherical polyacrylamide beads, which carry a negative surface charge representative of many natural environments. Ubiquitous, oppositely-charged ENPs - Au and Ag NPs - were synthesized and introduced into a flow cell subjected to a macroscopically uniform flow field via point source pulse injection, at three different flow rates. The negatively-charged ENPs behaved like a conservative tracer, in terms of spatio-temporal plume evolution. The positive AgNPs, however, displayed a decrease in their initially strong tendency to attach to the oppositely-charged porous medium. As a result, immobilization of the positive AgNPs was spatially and temporally limited to the vicinity of the point of injection; beyond this region, the AgNPs were mobile and effluent contained AgNPs with hydrodynamic diameters significantly larger than those of the injected AgNPs. This behavior is understood by dynamic light scattering and ζ potential measurements, which showed aggregation processes and inversion in particle surface charge to occur during transport of the positive ENPs. These findings have broad implications for ENP mobility and reactivity in the environment.