Aquitards can serve as long-term contaminant sources to aquifers when contaminant mass diffuses from the aquitard following aquifer source mass depletion. This study describes analytical and experimental approaches to understand reactive and nonreactive solute transport in a thin aquitard bounded by an adjacent aquifer. A series of well-controlled laboratory experiments were conducted in a two-dimensional flow chamber to quantify solute diffusion from a high-permeability sand into and subsequently out of kaolinite clay layers of vertical thickness 15 mm, 20 mm, and 60 mm. One-dimensional analytical solutions were developed for diffusion in a finite aquitard with mass exchange with an adjacent aquifer using the method of images. The analytical solutions showed very good agreement with measured breakthrough curves and aquitard concentration distributions measured in situ by light reflection visualization. Solutes with low retardation accumulated more stored mass with greater penetration distance in the aquitard compared to high-retardation solutes. However, because the duration of aquitard mass release was much longer, high-retardation solutes have a greater long-term back diffusion risk. The error associated with applying a semi-infinite domain analytical solution to a finite diffusion domain increases as a function of the system relative diffusion length scale, suggesting that the solutions using image sources should be applied in cases with rapid solute diffusion and/or thin clay layers. The solutions presented here can be extended to multilayer aquifer/low-permeability systems to assess the significance of back diffusion from thin layers.

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The occurrence of perchlorate in soybean sprouts (Glycine max L. Merr), water dropwort (Oenanthe stolonifera DC.), and lotus (Nelumbo nucifera Gaertn.) root, which are commonly consumed by people in South Korea, was determined by using an ion chromatograph coupled with a tandem mass spectrometer. For soybean sprouts (11 samples), perchlorate was detected in most (91%) of the samples at various concentrations of up to 78.4 μg/kg dry weight (DW); the mean concentration was 35.2 μg/kg DW. For water dropwort, of the 13 samples examined, four showed concentrations that were above the limit of quantification (LOQ). The mean perchlorate concentration was 20.7 μg/kg DW, and the highest perchlorate value was 39.9 μg/kg DW. Of the six lotus root samples examined, only one exhibited a detectable perchlorate concentration (17.3 μg/kg DW). For the accumulation experiments with artificially contaminated solutions, the concentrations of perchlorate in soybean sprouts gradually increased with the increase of perchlorate concentration in the solution. However, there was a decrease in the bioconcentration factor as the perchlorate concentration in the solution increased.

Solute diffusive exchange between low-permeability aquitards and high-permeability aquifers acts as a significant mediator of long-term contaminant fate. Aquifer contaminants diffuse into aquitards, but as contaminant sources are depleted, aquifer concentrations decline, triggering back diffusion from aquitards. The dynamics of the contaminant source depletion, or the source strength function, controls the timing of the transition of aquitards from sinks to sources. Here, we experimentally evaluate three archetypical transient source depletion models (step-change, linear, and exponential), and we use novel analytical solutions to accurately account for dynamic aquitard-aquifer diffusive transfer. Laboratory diffusion experiments were conducted using a well-controlled flow chamber to assess solute exchange between sand aquifer and kaolinite aquitard layers. Solute concentration profiles in the aquitard were measured in situ using electrical conductivity. Back diffusion was shown to begin earlier and produce larger mass flux for rapidly depleting sources. The analytical models showed very good correspondence with measured aquifer breakthrough curves and aquitard concentration profiles. The modeling approach links source dissolution and back diffusion, enabling assessment of human exposure risk and calculation of the back diffusion initiation time, as well as the resulting plume persistence.